The study investigated self-control, materialism, and need for achievement as predictors of cybercrime behaviour among youths in Ibadan metropolis. The study adopted ex-post factor research design while 200 youths in Ibadan metropolis were conveniently selected to respond to four validated questionnaires: Cybercrime Behaviour Scale, Brief Multidimensional Self-Control Scale, Materialistic Value Scale, and Need for Achievement Scale. Four hypotheses were tested using zero-order correlation, multiple regression, and t-test of independent sample. All hypotheses were accepted at a p <.05 level of significance. The result revealed that need for achievement [r (197) = .415, p < .05] and materialism [r (197) = .291, p < .05] had significant relationship with cybercrime behaviour, while self-control [r (197) = -.362, p <.05) inversely correlated with cybercrime behaviour. Also, the result indicated that self-control, need for achievement and materialism jointly predicted cybercrime behaviour [R² =.34, F (2,198) = 87.22, p <.05]. Furthermore, self-control [β =-.29, p <.05), need for achievement (β = .28, p <.05) and materialism (β =.51, p <.05) independently predicted cybercrime behaviour among the study participants. Finally, gender t (197) = 7.11, p < .05] and employment status F (2,197) = 4.49, p <.05) significantly influenced cybercrime behaviour among youths in Ibadan metropolis. The study concluded that self-control, need for achievement, materialism, gender, and employment status are strong predictors of cybercrime behaviour among youths in Ibadan metropolis. The study recommended that government should be proactive in meeting the needs of the youths to reduce cybercrime behaviour.