Background Patient-centered medical homes (PCMHs) may improve outcomes for non-elderly adults with mental illness, but the extent to which PCMHs are associated with preventive care and healthcare quality for this population is largely unknown. Our study addresses this gap by assessing the associations between receipt of care consistent with the PCMH and preventive care and healthcare quality for non-elderly adults with mental illness. Methods This surveillance study used self-reported data for 6,908 non-elderly adults with mental illness participating in the 2007–2012 Medical Expenditure Panel Survey. Preventive care and healthcare quality measures included: participant rating of all healthcare; cervical, breast, and colorectal cancer screening; current smoking; smoking cessation advice; flu shot; foot exam and eye exam for people with diabetes; and follow-up after emergency room visit for mental illness. Multiple logistic regression models were developed to compare the odds of meeting preventive care and healthcare quality measures for participants without a usual source of care, participants with a non-PCMH usual source of care, and participants who received care consistent with the PCMH. Results Compared to participants without a usual source of care, those with a non-PCMH usual source of care had better odds of meeting almost all measures examined, while those who received care consistent with the PCMH had better odds of meeting most measures. Participants who received care consistent with the PCMH had better odds of meeting only one measure compared to participants with a non-PCMH usual source of care. Conclusions Compared with having a non-PCMH usual source of care, receipt of care consistent with the PCMH does not appear to be associated with most preventive care or healthcare quality measures. These findings raise concerns about the potential value of the PCMH for non-elderly adults with mental illness and suggest that alternative models of primary care are needed to improve outcomes and address disparities for this population.