Globally, the number of small-scale miners (SSM) is estimated to be more than 25 million, but it supports the livelihoods of around 100 million individuals. In Tanzania, the number of SSM has increased from an estimated 150,000 in 1987 to ~1.5 million in 2017. The miners are at a high risk of occupational-related health challenges. The study aimed to assess the concentrations of respirable crystalline silica (RCS) and radon among the tanzanite mining communities in Simanjiro District, Tanzania. We carried out a cross-sectional study involving the Mererani mines in Tanzania. These are underground mines comprised of informally employed miners, i.e. SSM. Concentrations of RCS and radon gas were measured in 44 study units, i.e. 22 mining pits and within 22 houses in the general community, e.g. shops in the peri-mining community. A total of 132 respirable personal dust exposure samples (PDS), 3 from each of the study units were taken, but only 66 PDS from the mining pits were analysed, as this was the main interest of this study. Radon concentration was measured by continuous monitoring throughout the working shift (and overnight for residences) using AlphaGuard monitor. The medians and comparison to the reference values, OSHA USA PEL and WHO/IARC references, were done for RCS and radon, respectively, using SPSS Ver. 27.0.0). The median time-weighted average (TWA) concentration of the RCS in the mining pits was 1.23 mg/m3. Of all 66 personal dust samples from the mining pits, 65 (98.5%) had concentrations of RCS above the Occupational Safety and Health Administration (OSHA) permissible exposure limit (PEL) of 0.05 mg/m3. Mining pits had a median radon concentration of 169.50 bq/m3, which is above the World Health Organization (WHO)/International Commission on Radiation Protection (ICRP) recommended reference of 100.00 bq/m3 but not above the upper reference of 300.00 bq/m3, while the community buildings had a median radon concentration of 88.00 bq/m3. Overall, 9 (20.5%) and 17 (38.6%) radon measurements were above 300.00 bq/m3 and between 100.00 and 300.00 bq/m3 references, respectively. Specifically, in the mining pits, 9 (40.9%) test results were above 300.00 bq/m3, while none of the test results in the community was above 300.00 bq/m3. The tanzanite SSM in Mererani we highly exposed to RCS, which increases the risk of pulmonary diseases, including silicosis, tuberculosis, and pulmonary malignancies. Immediate action by OSHA Tanzania should be enforcement of wearing respirators by all miners throughout the working hours. Health education programmes to the SSM must be strengthened and OSHA Tanzania should adopt the 0.05 mg/m3 PEL, and enforce other occupational health and safety measures, including regular use of dust suppression mechanisms (water spray and wet drilling) and monitoring of RCS exposures among SSM. Monitoring of radon exposure both in the mining pits and community buildings should be conducted, and mitigation measures should be implemented in areas that exceed the reference level of 100.00 bq/m3.