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This study aims to identify the determinants of exhaustion of frontline and second-line healthcare workers (HCW) during the third wave of the COVID-19 pandemic. A case–control study was conducted based on an anonymously distributed questionnaire, which was completed by 1872 HCW. Exhaustion was assessed with a validated Romanian questionnaire. The Siegrist questionnaire was used to determine workload, reward and overcommitment. Frontline HCW reported significantly more frequent longer working hours (p = 0.0009) and a better perception of the management of the risk for infection (p = 0.0002) than second-line HCW. The effort and overcommitment scores were higher in frontline HCW (9.51 + 1.98 vs. 8.45 + 21, p < 0.001 and 16.34 ± 2.80 vs. 15.24 ± 2.94, p < 0.001, respectively) and the reward scores were lower (5.21 ± 1.522 vs. 5.99 ± 1.44, p < 0.001). In the fully adjusted regression model, age, imbalance between effort and reward, overcommitment and management of the risk of infection in the workplace were associated with the exhaustion score in each category of HCW. The number of working hours was correlated with exhaustion in frontline HCW and occupation in second-line HCW. There were more similarities than differences between frontline and second-line HCW. Even if frontline HCW had a higher risk of exhaustion, the risk was not negligible for all HCW.