Ultrafine particles produced by diesel-powered vehicles in underground mines are largely unaccounted for in mass-based air quality metrics. The Lung Deposited Surface Area concentration (LDSA) is an alternative to describe the harmfulness of particles. We aim to study concentrations and size distributions of LDSA at various locations in an underground mine as well as to evaluate the applicability of sensor-type measurement of LDSA. This study was conducted in an underground mine in Kemi, Finland, in 2017. Our main instrument was an electrical low-pressure impactor (ELPI+) inside a mobile laboratory. Additionally, five diffusion-charging based sensors were tested. The environment was challenging for the sensors as the particle size distribution was often outside the optimum range (20–300 nm) and dust accumulated inside the instruments. Despite this, the correlations with the ELPI+ were decent (R2 from 0.53 to 0.59). With the ELPI+ we determined that the maintenance area had the lowest mean LDSA concentration (79 ± 38 µm2 cm–3) of the measured locations. At the other locations, concentrations ranged from 137 to 405 µm2 cm–3. The mode particle size for the LDSA distribution was around 100 nm at most locations, with the blasting site as a notable exception (mode size closer to 700 nm). Diffusion-charging based sensors—perhaps aided by optical sensors—are potential solutions for long-term monitoring of LDSA if dust accumulation is taken care of. Our research indicates worker exposure could be reduced with the implementation of a sensor network to show which locations need either protective gear or increased ventilation.