Colloidal nanoplatelets (NPLs) have recently emerged as favorable light-emitting materials, which also show great potential as optical gain media due to their remarkable optical properties. In this work, we systematically investigate the optical gain performance of CdSe core and CdSe/CdS core/crown NPLs having different CdS crown size with one- and two-photon absorption pumping. The core/crown NPLs exhibit enhanced gain performance as compared to the core-only NPLs due to increased absorption cross section and the efficient interexciton funneling, which is from the CdS crown to the CdSe core. One- and two-photon absorption pumped amplified spontaneous emission thresholds are found as low as 41 μJ/cm2 and 4.48 mJ/cm2 , respectively. These thresholds surpass the best reported optical gain performance of the state-of-the-art colloidal nanocrystals (i.e., quantum dots, nanorods,etc.) emitting in the same spectral range as the NPLs. Moreover, gain coefficient of the NPLs is measured as high as 650 cm 1 , which is 4-fold larger than the best reported gain coefficient of the colloidal quantum dots. Finally, we demonstrate a two-photon absorption pumped vertical cavity surface emitting laser of the NPLs with a lasing threshold as low as 2.49 mJ/cm2 . These excellent results are attributed to the superior properties of the NPLs as optical gain media.