There is still limited data on the association between 25-hydroxyvitamin D (25(OH)D), parathyroid hormone (PTH), and bone health in healthy younger adults, particularly in Latin America. This cross-sectional analysis aimed to investigate the associations of 25(OH)D and plasma PTH concentrations with bone parameters, and potential confounders, in women living in a high (England) or low (Brazil) latitude country. Bone was assessed by either peripheral quantitative computed tomography (pQCT) (England) or dual-energy x-ray absorptiometry (DXA) scan (Brazil), serum 25(OH)D concentrations by high performance liquid chromatography tandem mass spectrometry (HPLC-MS) and PTH by the chemiluminescent method. In participants living in England, total volumetric bone mineral density (vBMD) was significantly higher in women <29 years compared to ≥30 years, and total and cortical vBMD values at the 66% site were negatively correlated with weight and body mass index (BMI). In participants living in Brazil, age was positively correlated with bone mineral density (BMD) at the femur and bone mineral content (BMC), and weight, BMI, and body fat were correlated with BMD (lumbar spine and femur) and BMC. PTH concentrations were negatively correlated with 25(OH)D concentrations, and the prevalence of secondary hyperparathyroidism was 28.6% (n = 14) in participants with concentrations <25 nmol/L and 12.2% (n = 41) with concentrations between 25 and 49.9 nmol/L, compared to 6.3% (n = 79) in those with concentrations ≥50 nmol/L. In conclusion, weight and BMI were significantly correlated with bone parameters in both groups and age was significantly correlated with BMD at the femoral neck for women living in Brazil only. Although 25(OH)D concentrations were not correlated to bone parameters at any sites, in either country, PTH concentrations showed a significant correlation with total vBMD at the 66% site for women living in England. Secondary hyperparathyroidism was more common amongst those with deficient and insufficient vitamin D status.