In 2007, the duo released their second studio album, Hook Me Up, which also peaked at number two in Australia and was certified 2× platinum for selling over 140,000 copies.

The album's title track, "Hook Me Up", was the Veronicas' first number one single in Australia,[2] while "Untouched" was an international top-ten hit, especially in Sweden, where it topped the chart for seven weeks.

In 2004, the sisters, who were then performing as "The Twins" (and who were being managed by their father Joseph Origliasso at that time), were introduced by Gabrielle McKinley to Robin Donald Smith.

These included Clif Magness (who has written with Avril Lavigne), Billy Steinberg (Madonna, Cyndi Lauper), Max Martin (Britney Spears, Katy Perry, P!nk), Eric Nova, Dead Mono and Vince DeGiorgio, where they created a catalogue of over 50 songs.

[10][failed verification] Multiplay also secured introductions and auditions for them with numerous recording companies, including Sony, EMI, Universal, BMG and Warner Music.

On their return to Australia, Smith and Bell met with the executives at Engine Room (a subsidiary of PBL (Packer) Group).

Seymour Stein and senior executives recognised that Smith and Bell had discovered and developed a musical talent, signing them quickly to a recording contract with Warner Bros. Records/Sire America, for a reported sum of two million dollars.

[13][14] Archie Comics had asked Warner Music Group to hand over all publicity rights and to pay US$200 million in damages.

The Secret Life of The Veronicas spent a year on the ARIA album chart without leaving the Top 40.

[30] Lisa and Jessica are the faces of Choice Calvin Klein[31] and Australian hair product company nu:u.

[36] The twins have also created a fashion line called "The Veronicas for Target" which was released in stores on 25 August 2007 in Australia.

[37][38] On 2 December 2006, The Veronicas released a CD/DVD, titled Exposed... the Secret Life of The Veronicas in Australia which features live performances from their Australian 2006 Revolution Tour and a DVD featuring parts of the sisters' live performances throughout 2005–2006, including footage that had previously not been seen, and their music videos.

The album was written and recorded in Los Angeles, California, with Toby Gad, Billy Steinberg, Greg Wells, Shelly Peiken and John Feldmann.

[46][47] The lead single from the album, "Hook Me Up", was added to Australian radio on 27 August 2007, but was physically released on 22 September 2007.

[75] Jessica Origliasso stated that the album was to be inspired by artists The Subways, The Dead Weather, Mazzy Star, Ladytron and Peaches.

[76][77][78][79] Lending their vocals elsewhere, Lisa and Jessica also collaborated with Michael Paynter to record a song called "Love the Fall" for his homonymous EP.

[83] Lisa also started a group called the Dead Cool Dropouts with her friend Tyler Bryant, mostly done using GarageBand on Mac.

It was later announced that a record deal had been struck with Sony Music Entertainment, and the long anticipated third album was set to be released late in 2014.

[94] On 31 October, during a special album release secret show, song "If You Love Someone" was announced as a second single.

[102] Social media users gave mixed responses during the night but there was praise for The Veronicas going topless on national television.

[106] The pair planned to release their next single, "Life of the Party" featuring Australian rapper Allday, in July 2019,[107] although this did not occur.

In October 2019, it was confirmed the duo's reality show, titled The Veronicas: Blood Is for Life, which premiered on MTV on 10 November 2019.

At their Melbourne date, the duo was preceded by a Facebook event titled "Wall of death when The Veronica's play Untouched at Good Things".

[111] In June 2020 the Sydney Morning Herald reported that The Veronicas were to fill as guest mentors for the ninth season of The Voice Australia coach Boy George, who would be mentoring his acts remotely from the UK because of travel restrictions in place due to the COVID-19 pandemic.

[124] In 2006, the Veronicas joined Steve Irwin's Wildlife Warriors Worldwide, a charity that deals with the protection of animals and their natural environments.

[128] Lisa also marched alongside Drew Barrymore, Pete Wentz, Janice Dickinson, and other celebrities in support of gay marriage in California at a May 2009 March in Los Angeles protesting 26 May 2009 decision of the California Supreme Court ruling upholding Proposition 8.

[130] In 2010 Lisa and Jessica were honoured as Wildlife Warriors of the year for their efforts in publicizing animal protection and conservation on a worldwide scale.

[136] On 27 January 2010 they announced via Twitter that they had signed a deal with cosmetic brand Flirt!, a division of Estée Lauder, to be the faces of their "Rock-n-Rebel" perfume.

[137][138] They became ambassadors for the fragrance with the deal to including a multi-million dollar promotion during mid-2010[139][140] which also included giving make-up tips via the Rock-n-Rebel website and judged a beauty contest where young women were asked to submit photos of their "ultimate rock star style".

"[143] The colours used for their fashion line include black and white and also features cherries, pirate motifs and love heart details.