This paper presents the preparation of different kinds of titanium oxide fractal structures on the surface of titanium by inverse pulsed laser deposition (IPLD) in air and water. In air, two-dimensional fractal structures are obtained with a low pulse energy. However, their branches units are aggregated and nanoscale branches disappear due to the high substrate temperature, causing the low fractal dimension of structure. When a higher laser energy is applied, the preformed deposited material forms a porous film, which reduces heat transfer from substrate. Therefore, three-dimensional and one-dimensional fractal structures with nanoscale branches on the topside of the film can be obtained. Then the desired two-dimensional fractal structures with nano-branches are obtained in water due to the water-induced rapid cooling of substrate temperature and plasma shock wave-induced particle’s expansion along the surface of substrate. Meanwhile, the asymmetry of fractal structure units analyzed by diffusion limited aggregation (DLA) model is caused by the difference of the distance between the initial deposited particles. In addition, when the pulse energy goes up to 111 mJ, the branches of two-dimensional fractal structure units are also aggregated and form isolated particles. The idea about modification of substrate temperature and water can guide the preparation of the desired titanium oxide fractal structures in pulsed laser deposition (PLD), which is also applicable to other materials.