Thermally conductive polymeric materials have attracted great interest from academia and industry for several decades. Herein, we report a facile method to fabricate BNNS/PP composites with excellent properties, especially the in-plane thermal conductivity. SEM and XRD results show the orderly dispersion and high orientation of BNNS along the in-plane direction. Attractively, the in-plane thermal conductivity of BNNS/PP composites after 20 times of folding and hot pressing is dramatically improved to 4.08 W/mk at a BNNS content of only 19.1 vol%, which is 20 times higher than that of pure PP and 480% higher than that of single hot pressing composite at the same filler content. In addition, The Hashin-Shtrikman (HS) model and finite element simulations are introduced to interpret the improvement of in-plane thermal conductivity of BNNS/PP composites after repeated hot pressing. Meanwhile, the influence of parallel orientation and layered distribution of BNNS on the mechanical and dielectric properties of BNNS/PP composites has been investigated. This facile method presents a novel approach to design and fabricate polymer composites with excellent in-plane thermal conductivity.