wt% Sn), are referred to as "liquid metals (LMs)" [1] because of their low melting points (near or even below room temperature). These materials have low toxicity, in contrast with well-known LM Hg, while possessing both high electrical conductivity (as "metals") and high fluidity (as "liquids"). [2] These characteristics afford high potential in a wide variety of cutting-edge technologies. [3][4][5][6][7][8][9][10] Although unmodified LMs are promising for various applications, [3,11,12] modification can extend the application scope. [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] LMs can be tailored into the form of colloidal microdroplets, [17][18][19][20][21][22][23][24][25][26][27] which enables their dispersion in another carrier liquid or in solidifiable matrices. Despite their high interfacial tension, the dispersed LM microdroplets can remain as discrete particles (without immediate coalescence) owing to the solid oxide layer that spontaneously forms on the outermost particle surface, [2] unless this layer is intentionally destroyed. [24,[28][29][30] This oxide layer, known to be mostly Ga 2 O 3 , [2,31] enables shape transformation of the LM microdroplets, [19][20][21] surface functionalization, [32][33][34][35] adhesion to substrates, [2,36,37] and templated synthesis of other particulate matter. [10] Intuitively, an oxide passivation layer with an ultrawide bandgap (≈4.8 eV) [18] may seem undesirable in applications where electrical percolation via the core metal phase of the microdroplets is important; however, the surface oxide layer may be useful in certain classes of applications where fine tuning of the dielectric properties or electrical breakdown strength of the electronic devices embedding LMs is required. [38,39] Furthermore, the electronic properties of the oxide skin, in conjunction with the core metal phase, are prospectively key factors in the photothermal conversion and photocatalytic activity of LM microdroplets, [17,18,40,41] with significant implications in human health and environmental applications such as targeted therapeutics [9,23,[42][43][44] and pollutant removal. [45] Thus, the unique tunability of the electronic properties by employing external oxide materials [17,18,[46][47][48] calls for follow-up research on various combinations of LMs and other particulate additives.LM microdroplets, when suspended as discrete particles with a solid oxide skin in a liquid medium, increase the viscosity (ɳ) of the resulting colloidal systems in a loading-dependent manner, and even induce elasticity at high loadings. [24,25,49,50] Such rheological properties of colloidal LM suspensions (or Ga and Ga-based alloys have recently received significant attention as "liquid metals (LMs)" with the combined advantages of a low toxicity, low melting point, high fluidity, and high conductivity. An important method for modifying LMs for enhanced processabilities and new applications is to tailor them into colloidal microdroplets suspended in a liquid medium. In this study, the unique vitri...