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Following a decade of professional acting, in 1994 Gilley started his own film making company, P.U.R.E. Productions.

In 1998, Gilley began to make the Peace One Day documentary, eventually deciding to aim for a UN resolution formalising the idea. This goal was reached in 2001 when UN GA resolution, put forward by the UK and Costa Rican Governments, was unanimously adopted to establish the first ever day of global cease fire and non-violence fixed in the calendar as 21 September annually. This resolution drew on a 1981 UN resolution that had declared the third Tuesday of September the international day of peace.

Gilley organised two concerts at Brixton Academy, London, on 21 September 2002 and 2003. In 2004, the Peace One Day documentary premiered at the Edinburgh Film Festival, then the BBC aired the documentary in September of the same year. On the other side of the Atlantic in 2005, Angelina Jolie and Jonny Lee Miller hosted the North American Film Premiere to highlight Peace Day.

In May 2006, the Peace One Day Citizenship Resource Pack was launched after conversations with over 30,000 young people and teachers. In 2007, a second edition of the Citizenship Resource Pack was made available to every secondary school in the UK.

Gilley produced and filmed The Day After Peace, in association with the BBC. The film documents the first ever life-saving activity on the day - polio vaccinations on 21 September 2007 in insecure regions of south and east Afghanistan. In May 2008 Jeremy Gilley received the award Campaigner of the Year.

In early September 2008 Gilley and Jude Law travelled to Afghanistan to screen The Day After Peace. 

On 21 September 2010, the Board of the Carnegie Foundation announced that Peace One Day and Jeremy Gilley would be the recipient of the Wateler Peace Prize. On 6 December 2011, Gilley was a founding signatory of the Pledge to Peace at the Peace and Well Being Conference at the European Parliament in Brussels. On 19th October 2011 Jeremy was awarded the IVCA Fellowship. 

He was also awarded the Cinema for Peace 2009 for the Most Inspirational Movie of the Year (The Day After Peace), the Cinema Vérité Award (The Day After Peace), Best Documentary Award (The Day After Peace) at the Zimbabwe Film Festival, Britain’s Best Award 2008 (Campaigner of the Year), IVCA Clarion Champion Award and was the recipient of the James Hammerstein Award in 2006.

Jeremy Gilley was a Counsellor at One Young World Summits: 2012 in Pittsburgh.