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Background: Globally 10% of women have an unmet need for contraception, with higher rates in sub-Saharan Africa. Programs to improve family planning (FP) outcomes require data on how service characteristics (e.g., geographic access, quality) and women's characteristics are associated with contraceptive use. Materials and Methods: We combined data from health facility assessments (2018 and 2019) and a population-based regional household survey (2018) of married and in-union women ages 15–49 in the Kigoma Region of Tanzania. We assessed the associations between contraceptive use and service (i.e., distance, methods available, personnel) and women's (e.g., demographic characteristics, fertility experiences and intentions, attitudes toward FP) characteristics. Results: In this largely rural sample (n = 4,372), 21.7% of women used modern reversible contraceptive methods. Most variables were associated with contraceptive use in bivariate analyses. In multivariate analyses, access to services located <2 km of one's home that offered five methods (adjusted odds ratio [aOR] = 1.57, confidence interval [CI] = 1.18–2.10) and had basic amenities (aOR = 1.66, CI = 1.24–2.2) increased the odds of contraceptive use. Among individual variables, believing that FP benefits the family (aOR = 3.65, CI = 2.18–6.11) and believing that contraception is safe (aOR = 2.48, CI = 1.92–3.20) and effective (aOR = 3.59, CI = 2.63–4.90) had strong associations with contraceptive use. Conclusions: Both service and individual characteristics were associated with contraceptive use, suggesting the importance of coordination between efforts to improve access to services and social and behavior change interventions that address motivations, knowledge, and attitudes toward FP. [ABSTRACT FROM AUTHOR]