Studies suggest both alexithymia and impulsivity (partially) explain aggressive behavior in traumatic brain injury (TBI) patients, but none of these studies use both questionnaire and performance‐based measures as recommended, nor simultaneously investigate both impulsivity and alexithymia. The available studies therefore likely miss part of the constructs of alexithymia and impulsivity, and do not comprehensively assess the mediating effects of both constructs in the relationship between TBI and aggression. A sample of N = 281 incarcerated individuals were recruited from Dutch penitentiary institutions, and completed the Buss Perry Aggression Questionnaire (aggression), BIS‐11 (impulsivity) and Toronto Alexithymia Scale‐20 (alexithymia) questionnaires, as well as a stop‐signal task and an emotion recognition paradigm. Several multiple mediation analyses were conducted using structural equation modelling, to assess the viability of a causal theoretical model of aggression. The final planned models were the original models with a good fit with the data (comparative fit index > 0.95, root mean square error of approximation and Standardized root mean square residual < 0.05), and results indicate that only questionnaire‐based impulsivity mediated the relationship between TBI and aggression. TBI was unrelated to alexithymia, stop‐signal or emotion recognition performance. Aggression was predicted by both alexithymia and impulsivity, but not by the performance measures. Post hoc analyses shows that alexithymia moderates the relationship between impulsivity and aggression. These results imply that aggressive incarcerated individuals showing impulsive behavior should be screened for TBI, since TBI is often overlooked or misdiagnosed, and indicate that both impulsivity and alexithymia are potential focus points for aggression reduction treatment in TBI patients.