Improving access to National Health Service (NHS) dentistry is a public health issue that has been a focus for successive governments and policy makers in the UK. To inform this process, commissioners of services need to understand trends in service use and demands of the local population. This study explored inequalities in dental services use among adults in a socially deprived, ethnically diverse metropolitan area of London; satisfaction with services; and public views for improvement of services. Data from 695 adults were analysed for this study (56% of the eligible sample). Inequalities in dental services use and satisfaction with care according to sociodemographic factors were assessed in unadjusted and fully adjusted models. The proportion of participants who reported attending the dentist in the last 24 months was 69%, with inequalities according to social grade, ethnicity, sex and age but not according to borough of residence. The most common areas identified by respondents for service improvement were availability of dentists, affordability of care, and accommodation of services. Among those who visited the dentist in the last 24 months, 90% were satisfied with the quality of care provided. However, there were inequalities in satisfaction with care according to borough and reason for the last dental visit.