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Background: Employment and income are important determinants of mental health (MH), but the extent that unemployment effects are mediated by reduced income is unclear. We estimated the total effect (TE) of unemployment on MH and the controlled direct effect (CDE) not acting via income. Methods: We included adults 25–64 years from nine waves of the UK Household Longitudinal Study (n = 45 497/ obs = 202 297). Unemployment was defined as not being in paid employment; common mental disorder (CMD) was defined as General Health Questionnaire-12 score ≥4. We conducted causal mediation analysis using double-robust marginal structural modelling, estimating odds ratios (OR) and absolute differences for effects of unemployment on CMD in the same year, before (TE) and after (CDE) blocking the income pathway. We calculated percentage mediation by income, with bootstrapped standard errors. Results: The TE of unemployment on CMD risk was OR 1.66 (95% CI 1.57–1.76), with 7.09% (6.21–7.97) absolute difference in prevalence; equivalent CDEs were OR 1.55 (1.46–1.66) and 6.08% (5.13–7.03). Income mediated 14.22% (8.04–20.40) of the TE. Percentage mediation was higher for job losses [15.10% (6.81–23.39)] than gains [8.77% (0.36–17.19)]; it was lowest for those 25–40 years [7.99% (−2.57 to 18.51)] and in poverty [2.63% (−2.22 to 7.49)]. Conclusions: A high proportion of the short-term effect of unemployment on MH is not explained by income, particularly for younger people and those in poverty. Population attributable fractions suggested 16.49% of CMD burden was due to unemployment, with 13.90% directly attributable to job loss rather than resultant income changes. Similar analytical approaches could explore how this differs across contexts, by other factors, and consider longer-term effects. [ABSTRACT FROM AUTHOR]