The study examined the associations of aldosterone-to-renin ratio (ARR), aldosterone concentration (PAC), and renin concentration (PRC) with adverse left ventricular (LV) remodeling in 56.4 ± 14.3-year-old Chinese participants (71% with hypertension) who underwent testing from September 2022 to March. Primary aldosteronism is a common cause of secondary hypertension associated with adverse LV remodeling. In multivariable analyses, one standard deviation of ARR significantly predicted left ventricular hypertrophy (LVH) with OR = 1.531 (95% CI 1.041–2.251, p = 0.030). The third tertile of ARR had a 6-fold higher risk of CHD compared to the first (2.1-050), especially in patients without mineralocorticoid receptor antagonists (MRA). A significant dose-response relationship was observed between ARR and CHD risk (p overall <0.001, p non-linear = 0.079). Increased ARR is associated with an increased risk of LV structural changes even below the clinical range of LV and may serve as an early marker. Earlier MRA treatment could be beneficial but requires confirmation in prospective studies.