Filtered cathodic vacuum arc (FCVA) is a promising technique for synthesizing extremely thin carbon films exhibiting highly tetrahedral (sp3) carbon atom hybridization. However, most FCVA studies are for incident ions impinging perpendicular to the substrate surface. In this study, the effects of the ion incidence angle on the thickness, structure, and surface roughness of amorphous carbon (a-C) films deposited under different substrate bias voltages were examined in the light of computational and experimental results. Dynamic simulations and film thickness measurements showed a decrease in film thickness with increasing ion incidence angle, attributed to the decrease in carbon ion fluence on the film surface. Carbon atom hybridization analysis revealed a critical ion incidence angle for a given substrate bias voltage. Simulation and experimental results demonstrated that the enhancement of sp3 hybridization resulted from carbon-carbon collision cascades on the growing film surface and densification induced by direct and recoil implantation processes controlled by the ion incidence angle and substrate bias voltage. The strong dependence of a-C film growth on the carbon ion incidence angle exemplified by the results of this study has direct implications in the oblique deposition of ultrathin a-C films with predominant tetrahedral carbon atom hybridization. The present study provides a framework for optimizing the ion incidence angle to achieve the deposition of a-C ultrathin films with high sp3 contents.