Increased stiffness of tissues has been recognised as a diagnostic feature of pathologies. Tissue stiffness characterisation usually involves the detection of tissue response from mechanical stimulation. Air-puff optical coherence elastography (OCE) can generate impulse surface acoustic waves (SAWs) on tissue surface without contact and evaluate the mechanical properties of tissue. This study endeavours to explore the optimal excitation angle for air-puff OCE, a parameter that lacks standardisation at present, by investigating the relationship between the frequency bandwidth and peak-to-peak signal-to-noise ratio (SNR) of SAWs for different excitation angles (relative to the normal surface) of air-puff on the sample, from 5° to 85°, with an interval of 5° applied on the phantom. Due to the unevenness of human hands, 20°, 45° and 70° angles were employed for human skin (10 healthy adults). The results show that a smaller excitation angle could produce higher wave frequency bandwidth; a 5° angle generated an SAW with 1747 Hz frequency bandwidth, while an 85° angle produced an SAW with 1205 Hz. Significant differences were not shown in peak-to-peak SNR comparison between 5° and 65° on the phantom, but between 65° and 85° at the excitation position, a reduction of 48.6% was observed. Furthermore, the group velocity of the SAWs was used to evaluate the bulk Young’s modulus of the human tissue. The outcomes could provide essential guidance for air-puff-based elastography studies in clinical applications and future tissue research.