Background and Aims: Resident satisfaction is a critical indicator of the quality of care in long-term care facilities (LTCFs). Yet, the relative importance quality of care factors in predicting resident satisfaction remains unclear for guiding resident support initiatives. This study aims to identify the relative contribution of personal and facility care service factors as predictors of satisfaction LTCF residents. Methods: This cross-sectional study enrolled a convenience sample of 399 older adult residents from LTCFs in Shanghai, Nanjing, and Changsha, China, from June to December 2023. The inclusion criteria were age 65 or older, fluency in speaking and reading simplified Chinese Mandarin, having resided in long-term care facilities for at least one month, and cognitive competence to comprehend the questionnaires. Hierarchical multiple regressions were utilized to examine self-report survey data on ten resident personal variables, and seven care facility service domains were examined for their relative contribution to resident care satisfaction. Moreover, the analysis included the interaction between personal factors and care service attributes. Results: The combined personal and care service factors explained 26.1% of the variance in overall resident satisfaction. Personal factors that predicted resident satisfaction included age, level of independence, and length of stay (ΔR² = 0.11). Of the care facility factors, the significant predictors of higher resident satisfaction were spending time (β = 0.60, p < 0.01, ΔR² = 0.09) and environment domains (β = 0.62, p < 0.01, ΔR² = 0.03). Age moderated the relationship between the spending time domain and overall satisfaction, with a positive effect for residents aged 70–79 compared to those aged 60–69 (β = −1.26, p < 0.05). Conclusions: This study provides evidence to suggest the importance of personal and care facility characteristics to LTFC resident satisfaction. Based on these findings, improved resident satisfaction is likely with LTCF care services that provide tailored care plans using resident characteristics.