While a high school student in Lincoln, Walcott played in several Lincoln-based bands, including Kid Quarkstar, with longtime friend and future Maroon 5 guitarist James Valentine.

After university, Walcott engaged in freelance recording, arranging, and performing work with a very wide variety of artists including the Chicago-based groups Las Guitarras de Espana, the Mighty Blue Kings, and Pinetop Seven.

He was also active in the improvisational and "experimental" music scene, performing with the likes of David Boykin, Mike Reed, and Keefe Jackson at such places as Fred Anderson's Velvet Lounge, the Hungry Brain, and the Green Mill, and also led his own group, the Nate Walcott Octet.

[1] While living in Chicago, both in college and after, Walcott remained connected to Nebraska, working as an arranger and player on records being produced by Mike Mogis for artists such as The Faint, Rilo Kiley, and Johnathan Rice.

While still a student and collaborating with musicians in the vibrant Lincoln and Omaha music scenes, Walcott met singer-songwriter Conor Oberst of the bands Bright Eyes, Commander Venus, and Desaparecidos.

In recent years, Walcott has done extensive freelance recording and arranging work, including with She & Him, U2, Beck, Jenny Lewis, First Aid Kit, Rilo Kiley, the Shins, and Maroon 5.

He has also maintained a busy freelance performing schedule with the likes of M. Ward, Eleni Mandell, The Living Sisters, Jonathan Wilson, Harper Simon, and Zavalaz, a new band led by Cedric Bixler-Zavala of The Mars Volta.