Carbon nanotube (CNT)−CNT contact and CNT distribution effects on anisotropic thermal transport in aligned CNT−polymer nanocomposites (PNCs) are studied using an off-lattice Monte Carlo numerical simulation. Inter-CNT contact and the associated thermal boundary resistance are shown here to significantly affect transport properties of PNCs, including anisotropy ratios. Previous studies have considered the effective thermal conductivities of CNT−PNCs using only a very large CNT−CNT thermal boundary resistance (TBR) compared to that of the CNT−matrix TBR as a limiting case. As CNT−CNT TBR is currently an unquantified parameter for CNT−polymer systems, and because it may be reduced by various techniques, heat transport with CNTs in contact is studied for a wide range of CNT−CNT TBR values, varying from 2 to 25 × 10−8 m2 K/W. The degree of CNT−CNT contact, CNT spatial distribution, and CNT−CNT TBR relative to CNT−matrix TBR are considered for 1−20% volume fraction of aligned single-walled and multi-walled CNTs...