Porque era a Pedra da Ressurreição e significava o "retorno" de sua família. Um meio de liberdade para um Dumbledore mais jovem e um meio de arrependimento para um Dumbledore mais velho. E no momento ele perdeu a cabeça e esqueceu que era uma Horcrux.
'The Resurrection Stone – to [Grindelwald], though I pretended not to know it, it meant an army of Inferi! To me, I confess, it meant the return of my parents, and the lifting of all responsibility from my shoulders.'
[...]
After another short pause, Harry said, ‘You tried to use the Resurrection Stone.’
Dumbledore nodded.
‘When I discovered it, after all those years, buried in the abandoned home of the Gaunts, the Hallow had craved most of all – though in my youth I had wanted it for very different reasons – I lost my head, Harry. I quite forgot that it was now a Horcrux, that the ring was sure to carry a curse. I picked it up, and I put it on, and for a second I imagined that I was about to see Ariana, and my mother, and my father, and to tell them how very, very sorry I was...
Deathly Hallows - Chapter 35: King's Cross
(ênfase minha)