Hypertension self-management is recommended for optimal blood pressure (BP) control, but self-identified residential contextual factors that hinder hypertension self-care are understudied. To quantify perceived neighborhood health and hypertension self-care and assess interactions with the area deprivation index (ADI) and healthy food availability at home. A cross-sectional study was conducted in Baltimore, Maryland, including primary care adults enrolled in the Achieving Blood Pressure Control Together trial between September 1, 2013, and June 30, 2014. Participants were Black and had at least 2 BP readings greater than or equal to 140/90 mm Hg in the 6 months before enrollment. Analyses were conducted from August 5, 2021, to January 28, 2022. Participants' perceived neighborhood health, defined as the mean standardized score across 4 subdomains of aesthetic quality, walkability, safety, and violence, with a higher score signifying better neighborhood health. Hypertension self-care behavior and self-efficacy. Multivariable generalized linear models were fit regressing each outcome on perceived neighborhood health (higher scores on each domain signify better perceived neighborhood health), adjusted for confounders, and interaction terms between neighborhood health and potential modifiers (ADI [higher percentiles correspond to more deprivation] and healthy food availability [higher scores indicate greater availability]) of the primary association were included. Among 159 participants (median [IQR] age, 57 [49-64] years; mean [SD] age, 57 (11) years; 117 women [74%]), median (IQR) hypertension self-care behavior was 50 (45-56) and self-efficacy was 64 (57-72). Better perceived neighborhood health was associated with greater hypertension self-care behavior (β, 2.48; 95% CI, 0.63-4.33) and self-efficacy (β, 4.42; 95% CI, 2.25-6.59); these associations persisted for all neighborhood health subdomains except aesthetic quality. There were no statistically significant interactions between perceived neighborhood health or its subdomains with ADI on self-care behavior (P = .74 for interaction) or self-efficacy (P = .85 for interaction). However, better perceived neighborhood aesthetic quality had associations with greater self-care behavior specifically at higher healthy food availability at home scores: β at -1 SD, -0.29; 95% CI, -2.89 to 2.30 vs β at 1 SD, 2.97; 95% CI, 0.46-5.47; P = .09 for interaction). Likewise, associations of perceived worse neighborhood violence with lower self-care behavior were attenuated at higher healthy food availability at home scores (β for -1 SD, 3.69; 95% CI, 1.31-6.08 vs β for 1 SD, 0.01; 95% CI, -2.53 to 2.54; P = .04 for interaction). In this cross-sectional study, better perceived neighborhood health was associated with greater hypertension self-care among Black individuals with hypertension, particularly among those with greater in-home food availability. Thus, optimizing hypertension self-management may require multifaceted interventions targeting both the patients' perceived contextual neighborhood barriers to self-care and availability of healthy food resources in the home.