Introduction: The sodium-to-potassium (Na:K) ratio in the diet is a critical biomarker for cardiovascular and metabolic health, yet global adherence to recommended levels remains poor. Objectives: The objective of this study was to identify dietary determinants of the dietary Na:K ratio and its associations with micronutrient intake and diet quality. Methods: An observational cross-sectional survey was conducted in a representative sample of manufacturing workers through a combined stratified proportional and two-stage probability sampling plan, with strata defined by company size and industrial sector from the state of Rio Grande do Norte, Brazil. Dietary intake was assessed using 24 h recalls via the Multiple Pass Method, with Na:K ratios calculated from quantified food composition data. Diet quality was assessed with the Diet Quality Index-International (DQI-I). Multiple linear regression was used to analyze associations of Na:K ratio with the study variables. Results: The survey was conducted in the state of Rio Grande do Norte, Brazil, in 921 randomly selected manufacturing workers. The sample mean age was 38.2 ± 10.7 years, 55.9% males, mean BMI 27.2 ± 4.80 kg/m2. The mean Na:K ratio was 1.97 ± 0.86, with only 0.54% of participants meeting the WHO recommended target (<0.57). Fast food (+3.29 mg/mg per serving, p < 0.001), rice, bread, and red meat significantly increased the ratio, while fruits (−0.16 mg/mg), dairy, white meat, and coffee were protective. Higher Na:K ratios were associated with lower intake of calcium, magnesium, phosphorus, and vitamins C, D, and E, as well as poorer diet quality (DQI-I score: −0.026 per 1 mg/mg increase, p < 0.001). Conclusions: These findings highlight the critical role of processed foods in elevating Na:K ratios and the potential for dietary modifications to improve both electrolyte balance and micronutrient adequacy in industrial workers. The study underscores the need for workplace interventions that simultaneously address sodium reduction, potassium enhancement, and overall diet quality improvement tailored to socioeconomic and cultural contexts, a triple approach not previously tested in intervention studies. Future studies should further investigate nutritional consequences of imbalanced Na:K intake.