The electroless deposition is an excellent method for the preparation of the CNTs with Ni-P layers. Pristine CNTs were ﬁrst oxygen-functionalized by treating them with a mixture of concentrated (HNO3 :H2SO4=1:3) acids. The SWNTs were obtained in the suspension of purification solution, In this work, the heat-treatment at 400°С transformed the amorphous Ni-P layer into the nanocrystalline Ni-P (crystalline Ni and Ni3P intermetallic compound) layer. The Ni-P-SWNTs before and after heat-treatment were studied using XRD and SAED. It is observed that the lattice parameters of Ni-P layers has difference from the bulk’s, indicting that the lattice change has taken place.