Arsenic (As) and mercury (Hg) are trace elements of major environmental and public health concern. Their relevance is due to their well-documented toxicological effects. In rapidly urbanizing port-industrial cities, soil contamination by these elements represents a critical challenge. This situation compromises sustainable urban development and environmental governance. This study had three main objectives: First, to evaluate the contamination status of As and Hg in urban soils using multiple geochemical indices; Second, to assess the potential human health risks associated with exposure in the urban environment of Talcahuano; Third, to identify the relative contributions of geogenic and anthropogenic sources based on spatial distribution patterns. A total of 420 soil samples were collected. These included 140 topsoil samples (TS; 0–10 cm), 140 subsoil samples (SS; 10–20 cm), and 140 deep-soil samples (DS; 150 cm). Arsenic concentrations were determined using hydride-generation atomic absorption spectrometry (HG-AAS). Mercury concentrations were measured by cold-vapour atomic absorption spectrometry (CV-AAS). Median As concentrations were 2.7 mg kg⁻¹ in TS, 3.1 mg kg⁻¹ in SS, and 2.5 mg kg⁻¹ in DS. The corresponding median Hg concentrations were 0.2 mg kg⁻¹ in TS and 1.4 mg kg⁻¹ in both SS and DS. Spatial distribution maps were generated through ordinary kriging interpolation. Geochemical baseline values were calculated using the median + 2 × MAD approach. The resulting baseline values were 7.8 mg kg⁻¹ for As and 3.6 mg kg⁻¹ for Hg. Contamination assessment was conducted using the geoaccumulation index (Igeo), enrichment factor (EF), and contamination factor (Cf). Results indicate that most soils are classified as uncontaminated. Enrichment levels were minimal and contamination factors were low. Nevertheless, isolated outliers were identified. These included one significantly enriched As sample and several moderately enriched or slightly contaminated Hg samples. Human health risk assessment incorporated the Hazard Index (HI) and Total Carcinogenic Risk (TCR). Results indicate that neither non-carcinogenic nor carcinogenic risks exceed acceptable thresholds at any investigated soil depth. Spatial analysis suggests that anthropogenic activities are the dominant sources of As and Hg in the study area. Traffic emissions and industrial activities appear to be the primary contributors.