Background: Nutritional metals (NM) are essential for neurodevelopment and cognitive performance during growth. Nevertheless, epidemiological evidence regarding the associations between NM and brain function remains understudied, particularly among adolescents. Therefore, the objective of this pilot study was to examine the effects of NM biomarkers such as iron (Fe), selenium (Se), zinc (Zn), magnesium (Mg), and copper (Cu) on neurobehavioral functions among a group of rural Bangladeshi adolescents. Methodology: We conducted a cross-sectional study involving 105 adolescents aged 13–17 from Araihazar, Bangladesh. Cognitive function was assessed using the computer-based Behavioral Assessment and Research System (BARS), focusing attention, memory, and executive function, and blood NM levels (Fe, Se, Zn, Mg, and Cu) were measured. Associations between individual minerals, NM composite scores, and cognition were analyzed using multiple linear regressions. Results: This study included 47 boys and 58 girls with an average age of 15 years. Fe levels were correlated with Continuous Performance Test (CPT) latency (r = −0.42, p < 0.05) and Se levels correlated with Match-to-Sample (MTS) correct count (r = 0.32, p < 0.01). Linear regressions showed that Se was associated with MTS correct count (b = 0.02, 95%CI: 0.01, −0.04), reflecting visual memory, and Fe was associated with CPT latency (b = −0.68, 95%CI: −1.11, −0.26), reflecting improved attention. The same BARS measures were also significantly associated with the 3-NM composite score. Conclusions: Our findings suggest that NM, particularly Fe, Se, and NM mixtures, could play a crucial role in brain development and neurocognitive function during adolescence. Further studies will help design national public health policies and strategies to address and mitigate brain health deficiencies among adolescents.