Molecular layer deposition (MLD) is a useful technique for fabricating hybrid organic-inorganic thin films. MLD allows for the growth of ultrathin and conformal films using sequential, self-limiting reactions. This article focuses on the MLD of hybrid organic-inorganic films grown using metal precursors and various organic alcohols that yield metal alkoxide films. This family of metal alkoxides can be described as “metalcones”. Many metalcones are possible, such as the “alucones” and “zincones” based on the reaction of trimethylaluminum and diethylzinc, respectively, with various organic diols such as ethylene glycol. Alloys of the various metalcones with their parent metal oxide atomic layer deposition (ALD) films can also be fabricated that have an organic-inorganic composition that can be adjusted by controlling the relative number of ALD and MLD cycles. These metalcone alloys have tunable chemical, optical, mechanical, and electrical properties that may be useful for designing various functional films. The metalcone hybrid organic-inorganic materials offer a new tool set for engineering thin film properties.