"Lord knows I’ve suffered heartache. But Daryl was by far the most painful of all," he writes of the actress, whom he dated in 2001 and who is currently married to Neil Young.
"Neil Young, I always loved you, but I’m afraid I hate you now," he adds.
Kilmer also reveals that he credits Crawford with helping him get through his 1996 divorce from Joanne Whalley, and shares that Jolie, whom he dated in 2004, is "perhaps the most soulful and serious" of all his past loves.
"When people ask what she’s like, I say she’s like other women and other superstars, just MORE," he writes.