Carbon nanotubes (CNTs) are promising materials because of their unique properties. However, the poor solubility in solvents limits the function of CNTs and hinders their applications in many fields. Surface modification of CNTs with polymers is an efficient method to solve this problem. Several polymers were tested for the preparation of CNT dispersions. In comparison with organic polymers, poly(organophosphazenes) are highly stable macromolecules with adjustable properties which depend on the side groups. This article is to describe the synthesis of thermally stable and soluble multi-walled CNT/poly(organophosphazene) composites. The poly(organophosphazene)s substituted with (a) 100 % quaternary protonated pyridinoxy (PPY), (b) 50 % quaternary protonated pyridinoxy and 50 % a long aliphatic chain alcohol (1-dodecanol) (PDK), and (c) 50 % quaternary protonated pyridinoxy and 50 % a glycol ether [(2-(2-methoxyethoxy)ethanol] (PET) have been synthesized. f-MWCNT/poly(organophosphazene) composites have been prepared by the treatment of the functionalized multi-walled carbon nanotubes (f-MWCNT) with the protonated polyphosphazenes (PPY, PDK, and PET) using different feed ratios [R (feed) = 1:1, 1:3, 1:5, 1:10 (w:w)]. The thermal stability of prepared composites (f-MWCNT/PPY, f-MWCNT/PDK, and f-MWCNT/PET) have been investigated by TGA. By considering thermal stabilities and solubility of all prepared composites, f-MWCNT/PPY1:5, f-MWCNT/PDK1:5, and f-MWCNT/PET1:5 have been chosen as optimum composite composition and characterized by P-31 NMR, H-1 NMR, XRD, Raman spectroscopy, and EDX analysis. The morphologic characterizations of the f-MWCNT/PPY1:5, f-MWCNT/PDK1:5, f-MWCNT/PET1:5 nanocomposites have been carried out by HRTEM. Excellent dispersions of the nanocomposites in water and common organic solvents have been achieved. The solubility and thermal stability of nanocomposites depend on the side groups on poly(organophosphazene).