The control of the morphologies and thus the optical, electrical, and magnetic effect of 2D thin films is a challenging task for the development of cost-efficient devices. In particular, the angular dependent magnetoresistance (MR) of surface thin films up to room temperature is an interesting phenomenon in materials science. Here, we report amorphous carbon thin films fabricated through chemical vapor deposition at a SiO2 substrate. Their structural and angular magnetoresistance properties were investigated by several analytical tools. Specifically, we used a physical property measurement system to estimate the magnitude of the angular MR of these as-prepared sample thin films from 2 K to 300 K. An angular MR magnitude of 1.6% for the undoped a-carbon thin films was found up to 300 K. Under the magnetic field of 7 T, these films possessed an angular MR of 15% at a low temperature of 2 K. A high disorder degree leads to a large magnitude of MR. The grain boundary scattering model was used to interpret the mechanism of this angular MR.