Considerable attention has been drawn to the use of volatile two‐terminal devices relying on the Mott transition for the stochastic generation of probabilistic bits (p‐bits) in emerging probabilistic computing. To improve randomness and endurance of bit streams provided by these devices, delicate control of the transient evolution of switchable domains is required to enhance stochastic p‐bit generation. Herein, we demonstrate that the randomness of p‐bit streams generated via the consecutive pulse inputs of pump‐probe protocols can be increased by the deliberate incorporation of metal nanoparticles (NPs), which influence the transient dynamics of the nanoscale metallic phase in VO2 Mott switches. Among the vertically stacked Pt‐NP‐containing VO2 threshold switches, those with higher Pt NP density show a considerably wider range of p‐bit operation (e.g., up to ∼300% increase in ΔVprobe upon going from (Pt NP/VO2)0 to (Pt NP/VO2)11) and can therefore be operated under the conditions of high speed (400 kbit/s), low power consumption (14 nJ/bit), and high stability (>105,200 bits) for p‐bit generation. Thus, our study presents a novel strategy that exploits nanoscale phase control to maximize the generation of nondeterministic information sources for energy‐efficient probabilistic computing hardware.This article is protected by copyright. All rights reserved