Carbon nanostructures were obtained by acetylene injection into an argon plasma jet in the presence of hydrogen. The samples were synthesized in similar conditions, except that the substrate deposition temperatures were varied, ranging from 473 to 973 K. A strong dependence of morphology, structure, and graphitization upon was found. We obtained vertical aligned carbon nanotubes (VA-CNTs) at low temperatures as 473 K, amorphous carbon nanoparticles (CNPs) at temperatures from about 573 to 673 K, and carbon nanowalls (CNWs) at high temperatures from 773 to 973 K. Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, elastic recoil detection analysis, X-ray photoelectron spectroscopy, and Raman spectroscopy were used to substantiate the differences in these material types. It is known that hydrogen concentration modifies strongly the properties of the materials. Different concentrations of hydrogen-bonded carbon could be identified in amorphous CNP, VA-CNT, and CNW. Also, the H : C ratios along depth were determined for the obtained materials.