Planetary ball milling (PBM) is a well-known technique for efficient size reduction and homogenization of materials that has been used for many decades in various engineering and industrial processes. More recently, it has emerged as a unique top-down nanofabrication approach for nanomaterials based on nanoscale grinding. However, its potential application in nanostructured thin film fabrication has not been fully explored, as only a limited number of studies have been carried out. In this work, the effects of different grinding parameters (speed, time and solvents) were used to create previously unstudied nanoscale grinding conditions for nanostructured thin film materials via PBM with distinct and novel properties: Nanoparticles of silicon, titanium disilicide (TiSi2) and zinc oxide (ZnO) ground in different solvents (deionized (DI) water/ ethylene glycol (EG)/isopropyl alcohol) resulted in colloidal suspensions (or nanoinks) that could be used to coat various substrates (wafers, glass, flexible substrates, etc.) via drop casting, doctor blading or dip coating. Thin film properties such as wettability, electrical conductivity and gas sensing behavior are studied. The fabricated thin film coating properties could be tuned depending on the combination of starting powder materials, grinding parameters and resulting nanoparticle size/geometry: The influence of surface chemistry, solvent type, particle geometry, surface roughness and defects was shown to alter the conductivity and surface wettability of the resultant films. Thus, thin films formed using PBM nanoinks allow varied and tunable properties for advanced multi-functional coatings and devices. To demonstrate the feasibility of PBM nanoinks for thin film device applications, ZnO nanoinks were used to create chemiresistive gas sensors that operate at room temperature. By varying grinding parameters (speed, time and solvent) thin film sensors with differing particle sizes and porosity were produced and tested with air/oxygen against hydrogen, argon and methane target gas species, in addition to relative humidity. Grinding speeds of up to 1000 rpm produced particle sizes and RMS thin film roughness below 100 nm, as measured by atomic force microscopy and scanning electron microscopy. Raman spectroscopy, photoluminescence and x-ray analysis confirmed the purity and structure of resulting films. The peak gas sensor response was found for grinding parameters of 400 rpm (average particle size 275 nm) and 30 minutes (average particle size 225 nm) in EG and DI water, respectively, which could be correlated to an increased film porosity and an enhanced electron concentration resulting from adsorption/desorption of oxygen ions on the surface of ZnO nanoparticles. Similarly, gas response and dynamic behavior were found to improve as the operating temperature was increased between 100 and 150 °C. These results demonstrate the use of low-cost PBM nanoinks to optimize the active materials for solution-processed thin film gas/humidity sensors that can operate at room temperature for use in environmental, medical, food packaging, laboratory, and industrial applications. Overall, the nanogrinding technique can produce large amounts of nanoparticle suspension with variable particle sizes for creating thin films with tunable properties. By adjusting grinding parameters, the nanoparticle shape/size and properties can be varied resulting in nanoparticle inks for inexpensive coatings on various substrates and for use in different applications. / Graduate