Eating away from home is a risk factor for poor diet quality and obesity. With an ever-increasing proportion of household food spend directed toward eating out, the proliferation of these food establishments may contribute to their use, a potential precursor to less healthy food choices and low overall diet quality. However few studies are conducted at the national level and across a range of away from home food sources. The purpose of this study was to examine the association between the density of away from home food establishments (e.g., restaurants, fast food outlets and cafés) and household spend on away from home food within a nationally representative sample for England, UK. A cross-sectional analysis of data from Wave 1 of the UK Household Longitudinal Survey (n = 24,047 adults aged ≥19y) was conducted. Exposure was characterised as the density of away from home food establishments to all other food sources within 1 mile of the home, divided into quintiles (Q1 as lowest exposure and Q5 as highest exposure). The primary outcome included households with a high away from home equivalised monthly food spend (≥25% of total food spend). Logistic regression was used to estimate associations between away from home food establishment exposure and high away from home food spend. Away from home food establishment density was significantly associated with a greater odds of high monthly food spend (Q3: OR = 1.18, 95% CI = 1.07, 1.30; Q4: OR = 1.30, 95% CI = 1.18, 1.43; and Q5: OR = 1.52, 95% CI = 1.37, 1.68) with attenuation after controlling for known socioeconomic confounders (Q4: OR = 1.13, 95% CI = 1.02, 1.25; and Q5: OR = 1.16, 95% CI = 1.04, 1.30) compared to those least exposed (Q1). Those most exposed to away from home food establishments had a 16% greater odds of allocating more than 25% of household food spend on away from home food sources. This study provides one of the first analyses at the national level to examine the role of the local food environment in relation to household food spend, a potential precursor to diet quality and health.