The quantitative and qualitative differences between the two-finger (TF) and two-thumb-encircling hands (TT) techniques were not sufficiently investigated to determine which is more effective for single-rescuer infant cardiopulmonary resuscitation (CPR). As the type of chest compression (CC) technique can impact survival rates and prognoses of patients, this study aimed to compare the adequacy of single-rescuer infant CPR CC techniques and explore participants’ CPR experiences using an exploratory sequential mixed methods design. To assess the adequacy of CC and ventilation according to technique, 70 students who completed basic life support provider certification among students from emergency medical services and nursing departments of a single college performed CC using the TF and TT techniques (4 sets of 5 cycles with a ratio of 30:2) in simulation. Meanwhile, a numeric rating scale was used to measure fatigue. SPSS (v. 25.0, IBM Corp, Armonk, NY, USA) was used to analyze the collected data by frequency analysis, descriptive statistics, paired t-test, and repeated measures analysis of variance (ANOVA). We conducted focus group interviews and analyzed CPR experiences. There were statistically significant differences between the TF and TT techniques in fatigue score (6.09 vs. 4.23 points, p < 0.001), average hands-off time (6.77 vs. 7.43 s, p =0.001), mean ventilation volume (41.40 vs. 35.51 ml, p = 0.002), CC accuracy rate (65.89% vs. 77.11%, p = 0.011), mean CC rate (104.37 vs. 107.11 beats/min, p = 0.020), overall CPR score (78.26 vs. 84.37 points, p = 0.005), and overall compression score (82.60 vs. 92.54 points, p < 0.001). Furthermore, we found significant differences over time in mean CC count (p = 0.030), mean ventilation volume (p = 0.042), and mean hands-off time (p = 0.029). Two categories (ambivalent attitudes and perception of pain) and five sub-categories were derived based on the results. In conclusion, as stated in the 2020 American Heart Association (AHA) guidelines, both TF and TT techniques are useful for single-rescuer infant CPR. Overall, TT technique provides higher quality of compressions at the cost of fewer ventilations. We recommend future studies of more diverse groups and techniques.