Books and other items are housed within the university's Craiglockhart campus.
The space has been revamped to mark 100 years since Craiglockhart Hydropathic was used as a hospital to treat shell-shocked officers during World War One.
A new bronze sculpture of Wilfred Owen has also been put on display.
As part of the relaunch, a light projection, paying tribute to the building's history during the Great War, will illuminate the facade of the campus building from Wednesday to Friday.
Sir Daniel is among five famous faces who have lent their voices to the poets collection.
The works of Owen's friend and mentor Siegfried Sassoon have been captured by actor Nathaniel Parker.Circumstances brought Owen and Sassoon together at Craiglockhart in the summer of 1917.
Poet, broadcaster and comedian Ian McMillan, journalist and broadcaster Allan Little and the award-winning author Dr Pat Barker have also recited works for a special recorded playlist.
Sir Daniel's association with Wilfred Owen's work stems back to his father, Poet Laureate Cecil Day-Lewis, who edited Owen's poetry in the 1960s. Sir Daniel's mother, Jill Balcon, was a vice-president of the Wilfred Owen Association.
Catherine Walker, collection curator, said: "Sir Daniel, Nathaniel, Allan, Ian and Pat have all given their time and expertise to support this project.
"Their distinctive voices have really brought the poems to life, giving our visitors an opportunity to hear and fully appreciate the poetry. We are extremely grateful to them."
Oscar-winning actor Sir Daniel Day-Lewis has recited seven of Wilfred Owen's most famous works to help relaunch Edinburgh Napier University's War Poets Collection.