The aim of this study was to develop acrylic matrix composites reinforced with one-dimensional (1-D) titanium dioxide (TiO2) micro and nano fillers that mimic the structure of enamel. To accomplish this, 1-D TiO2 was synthesized without surfactants or templates using a sol-gel assisted hydrothermal process. Two different approaches were investigated. One used titanium metal powder and yielded TiO2 rutile microrods. The other used titanium tetraisopropoxide (TTIP) and created TiO2 anatase nanorods. TiO2 morphology (size, aspect ratio and state of agglomeration) was affected by glycolic acid concentration and phosphate ion concentration for the titanium metal-based powders, and NaOH concentration for TTIP based powders. Composites were made with silanized TiO2 micro- and nano-rods in a 50:50 BisGMA:TEGDMA matrix. Organized composites made by injection molding or centrifuging and settling had more uniform mechanical properties (hardness, strength, Young’s modulus and toughness) than unorganized composites. Curing the composites under pressure reduced porosity enhancing mechanical behavior.