Monodisperse non-noble metal nanocrystals (NCs) that are highly uniform in shapes and particle size are much desired in various advanced applications,a nd are commonly prepared by either thermal decomposition or reduction, where reactive organometallic precursors or/and strong reducing agents are mandatory;however,these are usually toxic,costly, or suffer alackofavailability.Bulk Group 12 metals can now be converted into ligand-protected, highly crystalline,m onodisperse spherical metal NCs with precisely controlled sizes without using any precursors and reducers.T he method is based on low-power NIR-laser-induced size-selective layer-bylayer surface vaporization. The monodisperse Cd NCs show pronounced deep-UV (DUV) localized surface plasmon resonance making them highly competitive DUV-plasmonic materials.T his approach will promote appreciably the emergence of aw ide range of monodisperse technically important non-coinage metal NCs with compelling functionalities.Metal nanocrystals (NCs) are of particular importance in nanoscience and technology owing to their unique electrical, optical, magnetic,a nd catalytic properties,r endering them highly desirable in numerous state-of-the-art applications such as high-performance Li-ion batteries, [1] high-density renewable energy storage, [2] surface-enhanced Raman spectroscopy (SERS), [3] localized surface plasmon resonance (LSPR) sensors, [4] and theranostic probes. [5] To succeed in the above applications,m etal NCs in general ought to be made monodisperse with very narrow distribution in both dimension and morphology owing to the significant size and shape effects. [1,[5][6][7][8] Monodisperse colloidalm etal NCs have also been regarded as ideal building units for advanced superstructures and devices. [9] To date,s everal colloidal chemistry methods have been developed to synthesize monodisperse spherical metal NCs with controlled particle sizes. [1,[10][11][12] It is well-known that the colloidal chemistry is based on abottom-up strategy,where the neutral metal atoms need to be firstly released through either reduction or thermolysis of the precursors to initiate nucleation and subsequent growth of metal NCs.O wing to the intrinsic inertness,n oble metal NCs,s uch as Au and Pt, can be easily prepared by reduction of metal salts with alcohols. [10] In contrast, for the synthesis of non-noble metal NCs,r eactive organometallic precursors (that is,m etal carbonyls,m etal amides) or/and strong reducing agents (that is,superhydride, sodium borohydride) are prerequisite, [1,11,12] however, these are usually hazardous,c ostly,c omplex, and even lack availability.Herein, for the first time,wereport on arobust conversion strategy,f ree of precursors and reducing agents,w hich transforms bulk non-noble metals directly into ligand-protected, size-tailored, highly crystalline,m onodisperse spherical non-noble metal NCs,b yl ow-power nanosecond NIRlaser ablation/irradiation. This top-down route is distinct from what we developed previously for monodisperse quantum dots based on...