This study investigated the relationships among caregiving strain, coping, and mental health among caregivers of individuals with autism spectrum disorder (ASD) and the mediational moderation of caregiver needs. One hundred and ninety-three caregivers of individuals with ASD completed an online survey. Results showed that maladaptive coping behaviors were significant in mediating the relationship between strain and mental health. Professional service and emotional caregiving needs moderated the relationship between maladaptive coping and mental health at times of high caregiving strain, but not involvement, health information, and instrumental support needs. Results highlighted the negative effect of maladaptive coping, as well as professional service and emotional support needs were salient in moderating coping and mental health in times of high caregiving strain.