The direct integration of two-dimensional nanostructures into macroscopic porous carbon substrates is essential for their practical use in potential applications, which is a big challenge due to the difficulty of securing uniform coating layers. In this work, we demonstrate a very simple and effective method for the direct coating of MoS2 onto the surface of porous carbon structures having nano-sized pores, such as vertically aligned carbon nanotube arrays. A uniform coverage of MoS2 over carbon substrates was achieved by chemical vapor deposition of gaseous species derived from starting precursors in a closed reactor. Transmission electron microscopy images, X-ray diffraction data, and Raman spectra confirmed the formation of highly crystalline MoS2 layers. X-ray photoelectron and energy dispersive X-ray spectroscopies revealed highly uniform MoS2 layers over the whole surface of the carbon substrates. Our approach is also applicable for the synthesis of MoS2/carbon fiber paper (CFP) hybrid structures. The electrochemical tests showed that the as-synthesized MoS2/CFP structures can serve as highly active cathodes for reverse electrodialysis.