Few data are available on the association of high-sensitivity C-reactive protein (hs-CRP) and mortality independent of low-density lipoprotein (LDL) cholesterol in patients undergoing percutaneous coronary intervention (PCI). Consecutive patients (N = 8,834) undergoing PCI between October 28, 2002, and December 31, 2006, were followed through June 30, 2007 (average and maximum follow-up of 1.9 and 4.6 years, respectively). High-sensitivity CRP levels were classified into 4 groups: <1.0, 1.0 to 2.9, 3.0 to 9.9, and > or =10 mg/L. All-cause mortality rates were 14.4, 17.5, 25.7, and 56.4 per 1,000 person-years in patients with hs-CRP levels of <1.0, 1.0 to 2.9, 3.0 to 9.9, and > or =10 mg/L, respectively. Compared with patients with hs-CRP <1.0 mg/L, the hazard ratios of mortality after multivariable adjustment, including LDL cholesterol, associated with hs-CRP levels of 1.0 to 2.9, 3.0 to 9.9, and > or =10 mg/L were 1.27 (95% CI 0.91-1.75), 1.70 (95% CI 1.26-2.29), and 2.99 (95% CI 2.24-3.99), respectively (P trend < .001). After multivariable adjustment, trends of higher all-cause mortality at higher hs-CRP were present for patients with LDL cholesterol <70, 70 to 99, and > or =100 mg/dL (each P < .001). A test for interaction between LDL cholesterol and hs-CRP on all-cause mortality was not significant (P = .30). High-sensitivity CRP levels provide significant incremental prognostic information for all-cause mortality in long-term follow-up independent of LDL cholesterol.