The nonlinear optical response of CdSe and CdSe/CdS core/shell nanoplatelets (NPLs) in toluene suspension was determined by using Z-scan and optical Kerr gate (OKG) techniques at 800 nm in the femtosecond regime. First, an analysis of the nonlinearities based on the Z-scan resulted in n 2 = 1.4 × 10 −16 cm 2 /W and n 2 = 1.3 × 10 −16 cm 2 /W for CdSe and CdSe/CdS core/shell NPLs, respectively. Fifth-order nonlinear absorption behavior was predominant, resulting in α 4 = 4.0 × 10 −2 cm/GW for CdSe NPLs and α 4 = 9.0 × 10 −3 cm/GW for CdSe/CdS core/shell NPLs for an optical intensity of 60.97 and 122 GW/cm 2 , respectively. The nonlinear refractive index obtained from Z-scan is in good agreement with those obtained from the OKG, and the response time obtained from OKG showed a decay of less than 1 ps for all studied materials, about 5 times slower than the pulse duration. For optical intensities in the range between 30.45 and 182.8 GW/cm 2 , NLA was not observed for toluene but was observed for CdSe and CdSe/CdS core/shell NPLs, revealing that the presence of the NPLs decreases the threshold of the absorptive nonlinearity. The results are discussed and explained based on the well-known materials' electronic structure.Article pubs.acs.org/JPCC