She was a judge of Zee TV's singing reality show Sa Re Ga Ma Pa L'il Champs 2014.

[citation needed] Monali started her career in 2000 with the song 'Sundar Kato Sundar' from the Bengali movie Sajoni Aamar Sohag, sung along with Kavita Krishnamurti, Goutam Ghose and Pratik Choudhary.

[12] Joginder Tuteja of Bollywood Hungama picked it along with "Pehli Nazar Mein" as the biggest hits of the album and praised the song calling it "fresh, naughty and seductive".

That year, she collaborated with Pritam once again for the song "Meow", sung along with Suzanne D'Mello for the film Golmaal Returns.

Also, she performed the title track of Ekhane Aakash Neel, which is an official Bengali remake of the Hindi series Sanjivani, which aired on StarPlus.

[17][18] Her Bengali songs that year included releases such as 'It's Only Pyaar', 'O Yaara Ve', 'Bol Na Aar' from Dui Prithibi, 3 Tracks in Kellafate, and more.

In 2011, she sang songs like 'Naina', 'Ayo Manaye Jashn', 'Tik Tuk' from Rascals, 'Give it up' from United Six, 'Haal-e-dil' from Bbuddah... Hoga Terra Baap composed by Vishal–Shekhar, co-sung with Amitabh Bachchan.

In 2012, she sang 'Tu Mohabbat Hai' from Tere Naal Love Ho Gaya with Atif Aslam, composed by Sachin–Jigar, the song received critical acclaim.

[20] About the song she said: "I was feeling incomplete at the time as I had so much to offer, So, I would complain to Amit [Trivedi], saying what was the point of doing riyaaz [practice] for 10-12 hours if I cannot use it.

The song met with highly positive reviews, Filmfare wrote, "Monali Thakur instills sugar in our ears, the '50s orchestration, coupled with the perfect pitch of the singer manages to take you back to a bygone era",[22] while Mohar Basu of Koimoi wrote, "A romantic ballad out of the 50s, the song sung by Monali Thakur is astonishingly wonderful.

[24][25] Her next releases that year were 'Hip Hop Pammi' from Ramaiya Vastavaiya sung with Mika Singh, 'Muh Meetha Kara De' from Rabba Main Kya Karoon, 'Laila' from Nasha.

[26] 'Raghupati Raghav' from Krrish 3 was her next release, co-sung with Neeraj Shridhar and composed by Rajesh Roshan, the song received praise where singers were applauded for their energetic vocals.

[27] Her The following releases that year were 2 tracks from the movie I, Me Aur Main, 'Darbadar' in which she collaborated again with Sachin–Jigar and 'Meri Jaaniye' performed alongside Shaan.

Both of them were well appreciated by critics where, Suparna Thombare of 'Bollywood Life' stated about 'Darbadar' that "The ektara, clap sounds and Monali Thakur's silken voice lead you into this Sufi number that slowly zooms into a high energy song.

[29] She performed a female solo 'Laila' in Nasha, composed by musical duo Sangeet-Siddharth, the song was well received and called a sweet one.

In 2014, Thakur made her film debut with Lakshmi dealing with the harsh realities of human trafficking and child prostitution, which continues behind closed curtains in rural areas of India.

'Karthik' of Milliblog stated, "superbly led by Papon, till Ayushmann Khurrana and Monali Thakur interject later in the song with a lively melodic distraction".

According to her, "It doesn't happen often that in the world of EDMs and Hiphop Bollywood numbers one gets a chance to sing evergreen rich Indian melody, hence I can't thank Anu Ji enough to trust me as a singer with this beautiful song "Moh Moh Ke Dhaage", thus keeping a promise he made years back to me in a reality show where I was just a contestant".

[43] In 2018, Thakur appeared in the Zee5 show Lockdown along with Mickey Singh which was produced by Badshah's production house Afterhours.

[48][49] Apart from these Monali has also sung several super-hits like "Cham Cham" song from 2016 film Baaghi, which has garnered more than 1 Billion views on YouTube as of January 2022 and The Title Track of 2018 film "Badrinath Ki Dulhania", which she sang along with Neha Kakkar, Dev Negi and Ikka Singh, has been watched more than 800 Million times on Youtube as of January 2022.

As a child, she appeared in a Bengali television show, Aalokito ek Indu, in which she played the lead role Indubala.

Thakur made the marriage public only in June 2020 after releasing her single "Dil Ka Fitoor", which features her along with Maik.