A series of polytitanate nanobelt supported lean-burn NOx trap catalysts Pt-xK 2 CO 3 /K 2 Ti 8 O 17 with different weight loading of K 2 CO 3 (x = 0%, 5%, 15%, 20%, 25%, or 30%) were synthesized by successive impregnation. The nanobelt support K 2 Ti 8 O 17 displays a specific surface area as high as 302 m 2 /g, and the corresponding catalysts Pt-xK 2 CO 3 /K 2 Ti 8 O 17 show excellent NOx storage performance. As K 2 CO 3 loading increases from 5% to 30%, the NOx storage capacity (NSC) exhibits a volcano-type altering tendency with the maximum appearing at 25% (2.68 mmol/g); the highest NOx reduction efficiency of 99.2% was also achieved over this catalyst in cyclic alternative lean/ rich atmospheres. Further increase of K 2 CO 3 loading induces the formation of more bulk or bulk-like K 2 CO 3 species, decreasing the performance of the catalysts for NOx storage and reduction. HR-TEM and FT-IR results indicate that the K species exist as highly dispersed phases including K 2 O, K 2 CO 3 , and −OK groups, which are undetectable by X-ray diffraction (XRD) even at the K 2 CO 3 loading of 30%. Several carbonate species with different thermal stability and reactivity are identified by FT-IR and CO 2 -TPD. In situ diffuse reflectance FT-IR (DRIFTS) reveals that at low K 2 CO 3 loading (<20%) NOx is mainly stored as monodentate nitrates and monodentate nitrites, while at higher K 2 CO 3 loading NOx is mainly stored as bidentate nitrite species, which results from the decrease of oxidation ability of the catalysts due to the potential covering of K 2 CO 3 on Pt sites.