Background: Cardiovascular (CV) diseases are the leading cause of mortality globally. Reducing low-density lipoprotein cholesterol (LDL-C) is a proven strategy to decrease risk of acute CV events. The study aimed to estimate a PCSK9i-eligible population in Spain. Methods: We conducted a retrospective cohort study based on real-world data from the IQVIA Spanish Electronic Medical Records primary care database. Adult (≥18 y.o.) patients registered in the database between 2014 and 2020, diagnosed with myocardial infarction (MI), unstable angina (UA), ischemic stroke (IS), transient ischemic attack (TIA) or peripheral artery disease (PAD) and with at least 1 measurement of LDL-C or total cholesterol were included in the study and followed up for up to 12 months from the initial diagnosis. Results: The study included 9,516 patients; mean (SD) age was 67.7 (12.5) years, 63.9% were male and mean LDL-C was 117.3 (38.8) mg/dL. In the study population 28.5% of patients suffered an MI as most severe event during the study period, 10.0% had UA, 18.7% were diagnosed with IS, 13.6% with TIA, and 29.3% with PAD. At the time of last available LDL-C assessment (≥3 months after diagnosis), 64.4% of patients were on lipid lowering therapy (LLT). Of those, 45.4% were on high-intensity LLT (high-intensity statins with/without ezetimibe or PCSK9 inhibitors), 46.9% on moderate-intensity statins, and 7.7% on low-Intensity LLT (low-intensity statins, ezetimibe alone or non-statin LLT). Overall, 12.9% of treated patients achieved LDL-C levels <55 mg/dL; this proportion was the highest among those on high-intensity statins and any statin combined with ezetimibe (63.2%), followed by patients on moderate intensity statins (32.6%) and those on low-intensity LLTs (3.1%). A total of 17.1% of patients receiving optimized LLT had an LDL-C>100 mg/dL (LDL-C reimbursement threshold for PCSK9i in Spain). Conclusions: More than 85% of patients at very-high risk of cardiovascular events in our cohort do not achieve LDL-C <55 mg/dL recommended by 2019 ESC/EAS guidelines for management of dyslipidemia. More than 17% of the patients have LDL-C >100 mg/dL despite being treated with maximally tolerated LLT and, therefore, would be eligible for using PCSK9i within Spanish reimbursement criteria.