Hydrogenated amorphous carbon (a-C:H) films were deposited on the sidewall of 3-mm-wide stainless steel or Si trench, and the adhesion strength of the films was evaluated using a micro-scratch tester. Particularly, the effects of carbon ion implantation and Si-containing interlayer (a-SiCx:H) as the pretreatments on the adhesion strength of the a-C:H films prepared on the trench sidewall were investigated. It was found that both carbon ion implantation and interlayer improved the adhesion strength of the a-C:H films deposited on the trench sidewalls. In addition, the carbon ion implantation dominated the adhesion strength of the a-C:H films for the Si substrates, and the interlayer for the stainless steel substrates. In the case of the stainless steel substrates, the carbon was accumulated on the surface of the trench sidewall instead of implantation, whereas the carbon ions were implanted to the Si substrates on the trench sidewall to form a mixing layer. The a-SiCx:H interlayer forms Fe–Si bonds between the stainless steel substrate and the interlayer, which is thought to improve the adhesion strength. It was also found that there is a negative correlation between the trench depth and the adhesion strength regardless of the pretreatment methods.