AbstractCarbon fiber reinforced resin matrix composites, when subjected to multi‐angle delamination during vacuum hot pressing, suffered from defects such as uneven fiber distribution, resin‐rich zones, and voids. These defects caused varied damage and failure behaviors in the composites, seriously affecting their mechanical properties. In this paper, the defect distribution, tensile and flexural properties, and damage behaviors of multi‐angle lay‐up specimens prepared in an autoclave were studied. The results indicated that irregularly shaped voids in laminates with a 0° angle difference primarily led to local stress concentration. Elliptical and elongated voids in laminates with a 90° angle difference were mainly susceptible to delamination. The [0/90]8 layer exhibited the best overall mechanical properties. The proportion of 0° laminates had a direct impact on the mechanical properties, with 0° contact laminates on the bending‐compression side capable of withstanding higher bending loads. The [+45/−45]8 plyer demonstrated pseudo‐delayed behavior, enabling the laminate to show better toughness under load. Variations in damage due to the proportions and positions of the laminates influenced the mechanical properties and damages behavior of multi‐angle laminates.Highlights Angular differences were observed to affect void and resin distribution. The best overall mechanical properties were attributed to [0/90]8 laminates. Pseudo‐delay behavior was exhibited by [+45/−45]8 laminates. Proportion of 0° layers impacted mechanical properties. Greater bending loads were withstood by the 0° contact layer.