3799 www.MaterialsViews.com wileyonlinelibrary.com well as in providing a template for generating strong surface plasmon resonances (SPR). [12][13][14][15][16] They have also been used for a variety of sensing applications including chemical and biochemical sensors. [17][18][19][20][21] In principle, solid metals can be replaced by liquid metals to form "liquid metal"/"metal oxides" (LM/MO) structures. Interestingly, despite their immense potentials, LM/MO structures have rarely been reported. [ 22 ] Furthermore, none of these works take advantage of the nature of the incorporated liquid metals. In addition to the well-known benefi ts that solid metals can offer, liquid metals add extra dimensions to the structures, which originate from their soft and liquid nature. This brings fl exibility, the possibility of amalgamation with other metals and their recoverability, mobility and high conformation to the system.We have previously shown the possibility of coating relatively large liquid metal droplets of galinstan using metal oxide nanoparticles. [23][24][25] By doing this, we created liquid metal marbles with extraordinary physical and chemical properties. Our investigations associated these properties to the interfaces between liquid metal and metal oxide nanoparticles in combination with the fl exibility of the marbles, thereby providing extra degrees of freedom in order to manipulate their functionalities on demand. However, the properties of large liquid metal marbles are strongly surface dependent and the bulk of the droplet is mostly redundant. For using the bulk of liquid metals, it should be divided into the smallest possible stable entities.It has been demonstrated that sonication of bulk liquid metal droplets can produce micro-, meso-, and nanosized liquid metal spheres. Previous reports show that thiol-stabilized mercury and EGaIn (75 wt% Ga, 25 wt% In) liquid metal droplets with dimensions in the order of micro-to nanometer can be successfully synthesized through sonication. [ 26,27 ] In this work, we utilize micro-to nanosized galinstan spheres with coated metal oxide nanoparticles to form the LM/ MO spherical structures suspended in aqueous solutions. Galinstan (68.5 wt% Ga, 21.5 wt% In, and 10 wt% Sn) is chosen as it poses less health hazards in comparison to liquid metals such as mercury. The surface metal oxide nanoparticles are either inherently formed during the synthesis process or coated onto the surface of galinstan spheres. We fully characterize the LM/MO spherical structures in terms of stoichiometry and optical properties, including the demonstration of plasmon A new platform described as the liquid metal/metal oxide (LM/MO) framework is introduced. The constituent spherical structures of these frameworks are made of micro-to nanosized liquid metal spheres and nanosized metal oxides, combining the advantages of both materials. It is shown that the diameters of the spheres and the stoichiometry of the structures can be actively controlled. Additionally, the liquid suspension of these sphere...