Delirium is a serious and complex problem facing critically ill patients. This retrospective study aimed to explore the association between prognostic nutrition index (PNI) and delirium in critically ill patients in the intensive care unit (ICU). This study was based on the Medical Information Mart Intensive Care IV (MIMIC IV) database. Patients over 18 years of age were enrolled. Univariate and multivariate logistic regression analyses were performed to explore the association between PNI and delirium. Tendency analysis, subgroups analysis, and restricted cubic spline (RCS) were selected to further certify the association. The receiver operating characteristic curve (ROC) was adopted to assess the predictability of PNI to delirium. Propensity score matching (PSM) was used to reduce the interference of confounders. A total of 3,105 patients participated in this study. As the grade of malnutrition increases, the incidence of delirium increases in all models. The odds ratios (OR) of delirium in the fully adjusted model were 1.00 (reference), 1.04 (0.80, 1.36), 1.53 (1.17, 1.99), and 1.93 (1.44, 2.59). Strong U-shaped curves were found with RCS analysis between delirium and PNI in the subgroups of patients over 60 years of age and patients with chronic obstructive pulmonary disease (COPD). After PSM, the ORs of delirium were 1.44 (1.16, 1.79) and 1.53 (1.22, 1.93), respectively, in the univariate and multivariate logistic regression models. PNI is negatively associated with the prevalence of delirium in critically ill adults in the ICU. PNI is an independent risk factor for the incidence of delirium in adults in the ICU.