The control of local heterogeneities in metallic glasses (MGs) represents an emerging field to improve their plasticity, preventing the propagation of catastrophic shear bands (SBs) responsible for the macroscopically brittle failure. To date, a nanoengineered approach aimed at finely tuning local heterogeneities controlling SB nucleation and propagation is still missing, hindering the potential to develop MGs with large and tunable strength/ductility balance and controlled deformation behavior. In this work, we exploited the potential of pulsed laser deposition (PLD) to synthesize a novel class of crystal/glass ultrafine nanolaminates (U-NLs) in which a ∼4 nm thick crystalline Al separates 6 and 9 nm thick Zr50Cu50 glass nanolayers, while reporting a high density of sharp interfaces and large chemical intermixing. In addition, we tune the morphology by synthesizing compact and nanogranular U-NLs, exploiting, respectively, atom-by-atom or cluster-assembled growth regimes. For compact U-NLs, we report high mass density (∼8.35 g/cm3) and enhanced and tunable mechanical behavior, reaching maximum values of hardness and yield strength of up to 9.3 and 3.6 GPa, respectively. In addition, we show up to 3.6% homogeneous elastoplastic deformation in compression as a result of SB blocking by the Al-rich sublayers. On the other hand, nanogranular U-NLs exhibit slightly lower yield strength (3.4 GPa) in combination with enhanced elastoplastic deformation (∼6%) followed by the formation of superficial SBs, which are not percolative even at deformations exceeding 15%, as a result of the larger free volume content within the cluster-assembled structure and the presence of crystal/glass nanointerfaces, enabling to accommodate SB events. Overall, we show how PLD enables the synthesis of crystal/glass U-NLs with ultimate control of local heterogeneities down to the atomic scale, providing new nanoengineered strategies capable of deep control of the deformation behavior, surpassing traditional trade-off between strength and ductility. Our approach can be extended to other combinations of metallic materials with clear interest for industrial applications such as structural coatings and microelectronics (MEMS and NEMS).