Sherlock began her journalistic career as a freelancer, and has spoken on the importance of building community with locals when working as an on the ground freelancer.[1][6] She was working in the West Bank and Israel when she received word of unrest in Egypt. She traveled to Cairo, and reported from there on the 2011 Egyptian revolution before moving on to cover Libya's civil war.[1] Her work in Libya was her first time working in a conflict zone. During her time in Libya, she filed stories with the Los Angeles Times and The Sunday Times.[7]
In 2012, she won The Press Awards' Young Journalist of the Year award[8] and was hired by The Daily Telegraph[1][7] as their Middle East Correspondent.[9] While working for The Daily Telegraph, Sherlock covered the Syrian civil war. She reported on the Queiq River Massacre in January 2013.[10] She met American aid worker Kayla Mueller in 2013, and followed her work up until Mueller was kidnapped by the Islamic State in August 2013.[11] In 2014, Sherlock survived an attempted kidnapping herself while working in Yabrud.[12]
In early 2015, Sherlock was made a U.S. editor for The Daily Telegraph. During her time that position, she covered the 2016 presidential election.[9]
By 2019, Sherlock was working as an international correspondent for NPR. Her work with NPR has included covering stories relating to the Islamic State, and specifically relating to the women and children left behind by the group.[12]
In 2019, Sherlock's reporting was used for the short series "How it Ends" on NPR podcast Embedded. The short series covered four families searching for members who had joined the Islamic State.[12] The series was shortlisted for the Livingston Award in 2020.[9]