Carlton independently produced her next two albums, Rabbits on the Run (2011) and Liberman (2015),[1][2][3] which were acclaimed by critics for both its personal subject matter and departure from her previous musical style.

She later moved to New York City, where she attended Columbia University for one year before dropping out[14] and had a stint as a waitress in Hell's Kitchen.

Other unreleased tracks from her early demo tapes include "Faces", "Meggie Sue", "Little Mary", "Burden", "Wonder", "Devil Dance", and "Last Fall".

After hearing Carlton's demo of "A Thousand Miles", A&M president Ron Fair organized recording sessions and produced and arranged the song himself.

Carlton played piano and sang vocals; other instrumentation included a backing band, a 60-piece orchestra and sitar on "Paint It Black".

She provided the descant vocals for the Counting Crows version of the Joni Mitchell song "Big Yellow Taxi", played piano for Italian singer Zucchero, along with Haylie Ecker on violin for the song "Indaco Dagli Occhi Del Cielo",[25] and provided backing vocals for "Moving On" by Kimya Dawson for her album Hidden Vagenda.

[32] A single, "White Houses", released to radio in late August 2004, peaked at number 86 on the Billboard Hot 100.

[33] MTV censored and later banned the single's music video because of a controversial lyric in the song that refers to sexual intercourse.

Carlton attributed the censoring of the song to the Super Bowl XXXVIII halftime show controversy involving Janet Jackson which had occurred earlier that year.

[37][38] In the same period she collaborated with the Italian singer Zucchero Fornaciari featuring his song Indaco Dagli Occhi Del Cielo (cover of the well known Everybody's Got to Learn Sometime), together with the violinist Haylie Ecker, in the album Zu & Co.

[45] Second single "Hands on Me" was sent out to radio in February 2008 and reached number 30 on Billboard's Adult Top 40 Tracks chart.

On behalf of the charity Cape Farewell, they worked alongside researchers for the purpose of studying climate change.

[49] Carlton had been a part for PETA's Animal Birth Control Campaign;[50] she owns a long haired dachshund named Lord Victor.

Carlton's fourth studio album Rabbits on the Run was released on July 26, 2011, under Razor & Tie, the third record label she signed with,[51] and received praise from music critics who particularly noted its "strikingly personal" subject material.

The dreamy, fantastical sound of the album was achieved by recording direct to tape and features production by Steve Osborne.

[59] On September 19, a tweet on Carlton's account made by her management stated that "I Don't Want to Be a Bride" would be the next single off the record.

[61] The EP consists of four tracks, two of which are acoustic versions of Carlton's songs Hear the Bells and A Thousand Miles.

[62] Carlton announced in late 2012 that she had returned to Real World Studios to commence work on a new album with a theme of euphoria.

On a small tour in late 2013, Carlton teased new songs "Willows", "House Of Seven Swords", "A Matter Of Time", "Take It Easy" and "Unlock The Lock".

She performed a track titled "Willows" to promote the events for Fox New York TV, which she said was about the trees she had loved when she was growing up, and she revealed that Liberman would be released in 2015.

[64] In an interview with CBS News published on June 11, 2014, Carlton described the album as "kind of lush, trippy and beautiful...You really feel like you're falling into a rabbit hole of sounds."

[65][66] Writing for The Boston Globe, Ken Capobianco said the material "finds her a long way from 'A Thousand Miles' – and in a better place, artistically.

"[67] Matthew Schnipper of Pitchfork wrote that "Carlton's voice is the key attraction on songs [from Liberman] that register between low-key pop, rock, and folk.

[74][65] In May 2019, Carlton was announced to be making her Broadway debut with a lead role in the Carole King musical Beautiful, performing for a limited season from June 27.

[77] On May 27, 2019, Carlton announced via Instagram that her sixth album, produced by Dave Fridmann, was to be titled Love is an Art.

"[81] During 2024 Vanessa & her husband John Joseph McCauley III of the band 'Deer Tick' created the score for the upcoming film 'Wish You Were Here'.

In 2005, Carlton completed the New York City Marathon and donated the pledge money she collected to Musicians on Call, a nonprofit organization that brings live and recorded music to patients' bedsides.

"[84] On October 9, 2013, at a live performance in Bay Shore, New York, Carlton announced that she was expecting her first child with her fiancé John McCauley (of the band Deer Tick).

[87] On June 26, 2014, Carlton announced via Facebook that the release of Liberman would be delayed until the summer of 2015 because she was expecting a child with McCauley.