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Due to the incapability of one-dimensional (1D) and two-dimensional (2D) models in simulating the frontal polymerization (FP) process in laminated composites with multiple fiber angles (e.g., cross-ply, angle-ply), modeling a three-dimensional (3D) domain, which is more representative of practical applications, provides critical guidance in the control and optimization of the FP process. In this paper, subroutines are developed to achieve the 3D modeling of FP in unidirectional and cross-ply carbon fiber laminates with finite element analysis, which are validated against the experimental data. The 3D model is employed to study the effect of triggering direction in relevance to the fiber direction on the FP process, which cannot be studied using traditional 1D/2D models. Our findings suggest that triggering in the fiber direction leads to a higher front velocity, in comparison to cases where front was triggered in the direction perpendicular to the fiber. Moreover, the average front velocity in cross-ply laminates is on average 20~25% lower than that in unidirectional laminates. When triggered using two opposite fronts in the in-plane direction, the maximum temperature of the thermal spike in the cross-ply laminate, when two fronts merge, is about 100 °C lower than that in the unidirectional laminate. In cross-ply laminates, a sloped pattern forms across the thickness direction as the front propagates in the in-plane direction, as opposed to the traditionally observed uniform propagation pattern in unidirectional cases. Furthermore, the effect of thermal conductivity is studied using two additional composite laminates with glass (1.14 W/m·K) and Kevlar fibers (0.04 W/m·K). It is shown that the frontal velocity, degree of cure, and the thermal spike temperature decrease as the thermal conductivity reduces.