The Sarajevo Canton Winter Field Campaign 2018 (SAFICA) was a project that took place in winter 2017–2018 with an aim to characterize the chemical composition of aerosol in the Sarajevo Canton, Bosnia and Herzegovina (BiH), which has one of the worst air qualities in Europe. This paper presents the first characterization of the metals in PM10 (particulate matter aerodynamic diameters ≤10 μm) from continuous filter samples collected during an extended two-months winter period at the urban background Sarajevo and remote Ivan Sedlo sites. We report the results of 18 metals detected by inductively coupled plasma mass spectrometry (ICP-MS) and electrothermal atomic absorption spectrometry (ETAAS). The average mass concentrations of metals were higher at the Sarajevo site than at Ivan Sedlo and ranged from 0.050 ng/m3 (Co) to 188 ng/m3 (Fe) and from 0.021 ng/m3 (Co) to 61.8 ng/m3 (Fe), respectively. The BenMAP-CE model was used for estimating the annual BiH health (50% decrease in PM2.5 would save 4760+ lives) and economic benefits (costs of $2.29B) of improving the air quality. Additionally, the integrated energy and health assessment with the ExternE model provided an initial estimate of the additional health cost of BiH’s energy system.