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Abstract Wolf 359 (CN Leo, GJ 406, Gaia DR3 3864972938605115520) is a low-mass star in the fifth-closest neighboring system (2.41 pc). Because of its relative youth and proximity, Wolf 359 offers a unique opportunity to study substellar companions around M stars using infrared high-contrast imaging and radial velocity monitoring. We present the results ofMs-band (4.67μm) vector vortex coronagraphic imaging using Keck-NIRC2 and add 12 Keck-HIRES and 68 MAROON-X velocities to the radial velocity baseline. Our analysis incorporates these data alongside literature radial velocities from CARMENES, the High Accuracy Radial velocity Planet Searcher, and Keck-HIRES to rule out the existence of a close (a< 10 au) stellar or brown dwarf companion and the majority of large gas giant companions. Our survey does not refute or confirm the long-period radial velocity candidate, Wolf 359 b (P∼ 2900 days), but rules out the candidate's existence as a large gas giant (>4M_Jup) assuming an age of younger than 1 Gyr. We discuss the performance of our high-contrast imaging survey to aid future observers using Keck-NIRC2 in conjunction with the vortex coronagraph in theMsband and conclude by exploring the direct imaging capabilities with JWST to observe Jupiter- and Neptune-mass planets around Wolf 359.