Ibuprofen is a kind of nonsteroidal anti-inflammatory drug (NSAIDs), and it is considered to possess some antitumor effect. In this study, a novel nanomicellar carrier based on PEG-derivatized ibuprofen, PEG2K-Fmoc-Ibuprofen (PEG2K-FIbu), was developed for delivery of anticancer agents such as paclitaxel (PTX). This conjugate readily forms stable mixed micelles with PTX with a relatively high PTX loading capacity of 67%. The release of PTX from PTX-loaded PEG2K-FIbu micelles was significantly slower than that from Taxol formulation. PTX-loaded PEG2K-FIbu micelles and Taxol showed a comparable in vitro cytotoxicity. Importantly, PTX-loaded PEG2K-FIbu micelles demonstrated a much more pronounced in vivo therapeutic efficacy compared with Taxol with respect to both inhibition of tumor growth and animal survival. Our system may represent an attractive dual-functional delivery system to achieve synergistic activity with PTX while minimizing the carrier-associated toxicity.