 Muna 1965, Altafini akabatana neNapoli, nekuda kwekusawirirana kwake naAmarildo naPaolo Ferrario kuMilan, kwaakaumba hukama hunoshamisa hwekurwisa neItaly-Argentina mutambi wemutambo Omar Sivori, uyo aive shamwari yake yeItaly mu1962 World Cup muChile. Akaramba ari mukirabhu kwemakore manomwe, kusvikira muna 1972. Musi waDecember 31, 1967, mumutambo we2x2 wekurwisa Torino, Altafini akarova chinangwa cheacrobatic kubva kubhasikoro, golaço iyo yakamuita mukurumbira zvikuru nevateveri veNapoli. Munguva yake yekirabhu, akabatsira Napoli kukwikwidza zita nguva dzose, uye akakwanisa kutungamira Napoli kune yavo yakanakisa Serie A kupedzisa kusvika panguva iyoyo, achivabatsira kupedza wechipiri mu1967-68 Serie Amumwaka, achitevera kirabhu yake yekare yeMilan, achipedzisawo semutambi wechipiri wepamusoro muSerie A mwaka iwoyo. Akavabetserawo kupedza vari panzvimbo yechitatu muna 1966 na 1971. Mumwaka wa1971-72, Altafini akabatsirawo Napoli kuenda kumagumo eCoppa Italia ya1971-72, kunyangwe ivo vakakundwa 2-0 nekirabhu yake yapfuura, Milan. Pasinei nebasa rake munhoroondo yekirabhu, panguva yake kuNapoli, Altafini akakwanisa kuhwina mukombe mudiki, iyo Coppa delle Alpi, mumwaka wa1966-67. 