Low-cost optical particle counters effectively measure particulate matter (PM) mass concentrations once calibrated. Sensor calibration can be established by deriving a linear regression model by performing side-by-side measurements with a reference instrument. However, calibration differences between environmental and occupational settings have not been demonstrated. This study evaluated four commercially available, low-cost PM sensors (OPC-N3, SPS30, AirBeam2, and PMS A003) in both settings. The mass concentrations of three aerosols (salt, Arizona road dust, and Poly-alpha-olefin-4 oil) were measured and compared with a reference instrument. OPC-N3 and SPS30 were highly correlated (r = 0.99) with the reference instrument for all aerosol types in environmental settings. In occupational settings, SPS30, AirBeam2, and PMS A003 exhibited high correlation (>0.96), but the OPC-N3 correlation varied (r = 0.88–1.00). Response significantly (p < 0.001) varied between environmental and occupational settings for most particle sizes and aerosol types. Biases varied by particle size and aerosol type. SPS30 and OPC-N3 exhibited low bias for environmental settings, but all of the sensors showed a high bias for occupational settings. For intra-instrumental precision, SPS30 exhibited high precision for salt for both settings compared to the other low-cost sensors and aerosol types. These findings suggest that SPS30 and OPC-N3 can provide a reasonable estimate of PM mass concentrations if calibrated differently for environmental and occupational settings using site-specific calibration factors.