Palliative Care Day Services (PCDS) provide multidisciplinary support for individuals living with advanced or terminal illnesses. Although their use has expanded across the UK, limited empirical evidence exists on their cost implications and overall impact. Understanding their value is crucial to guide informed resource allocation in health and social care. This study investigates the financial and outcome-related aspects of three PCDS models implemented in England, Scotland, and Northern Ireland. A pragmatic, before-and-after cohort design was used to evaluate participants referred to PCDS between June 2017 and September 2018. Data on service use and related expenditures during the four weeks prior to attendance were collected using adapted Client Service Receipt Inventory (CSRI) tools. Costs per participant per day, alongside the monetary value of volunteer involvement, were calculated. Participant outcomes were assessed using the McGill Quality of Life–Expanded (MQOL-E), EQ-5D-5L, and ICECAP-Supportive Care Measure (ICECAP-SCM) instruments. Thirty-eight participants provided complete data at baseline and four weeks (centre 1: n = 8; centre 2: n = 8; centre 3: n = 22). Daily costs per participant ranged from £121–£190 without, and £172–£264 with, volunteer contributions. Volunteers accounted for 28–38% of the total cost of delivering PCDS. Across all centres, changes in mean costs and outcomes after four weeks were not statistically significant: total costs (centre 1: £570; centre 2: −£1127; centre 3: £65), MQOL-E (−0.48; 0.01; 0.24), EQ-5D-5L (0.05; 0.03; −0.03), and ICECAP-SCM (0.00; −0.01; 0.03). Scenario modelling indicated that unit costs per attendee could nearly double if attendance levels were constant between centres. Volunteers represent a substantial and often under-recognized component of PCDS delivery costs. However, across the three UK configurations studied, no conclusive evidence was found for improvements in cost efficiency or participant outcomes. The study outlines methodological insights and proposes directions for future evaluations of PCDS cost-effectiveness.