modulators, [14,15] and photodetectors. [16][17][18][19][20] The combination of a broadband lightabsorption range (from far-infrared to ultraviolet ranges in theory [21] ) and ultrahigh carrier mobility (1 000 000 cm 2 V −1 s −1 in experiment [22] ) makes graphene a star contender for photodetection applications. [16][17][18][19][20]23] The first reported spatial graphene photodetector (GPD) achieved a bandwidth of ≈40 GHz, and the ultrahigh intrinsic operation speeds could be well over 500 GHz, surpassing state-of-the-art PDs based on other materials. [16] However, the uniform 2.3% optical absorption of graphene limits the photoresponsivity of GPDs to several mA W −1 . [16,17] To enhance the optical absorption of graphene and thus the photoresponsivity of GPDs, microcavities, [24] plasmon resonators, [25] and silicon optical waveguides [18][19][20]26,27] have been utilized, but these structures weaken the broadband characteristic of GPDs. Another method carried out by fabricating a hybrid photodetector consisting of graphene covered by a thin film of colloidal quantum dots greatly improves the photoresponsivity from visible to near-infrared ranges. [28] However, the operation stability of this kind of GPD may not be satisfactory due to the air instability of colloidal quantum dots and the "dirty" interface between graphene and the cover layer. Moreover, colloidal quantum dots cannot be obtained with complementary metal-oxide-semiconductor (CMOS)-compatible fabrication processes, which are critical for low-cost devices. Hence, new methods should be proposed to achieve a CMOS-compatible broadband GPD with high photoresponsivity and high operation stability.TiO 2 nanomaterials have attracted considerable attention for applications in optoelectronic devices, [29] solar cells, [30] and photocatalysts [31] due to their advantages such as nontoxicity, low cost, chemical and thermal stability, and resistance to photocorrosion. [32][33][34] TiO 2 nanomaterials have been widely used as a shielding layer to prevent penetration of water molecules and oxygen gas. [35,36] Thus, thin TiO 2 films with low gas permeabilities can be excellent protection layers for graphene in high-stability GPDs. TiO 2 has three polymorphs: rutile, anatase, and brookite. [37] The metastable anatase form shows better performance in energy-related applications and optoelectronics because its formation temperature is relatively low and numerous intrinsic point defects exist in incomplete lattices. [38] Photodetectors Graphene, a single sheet of carbon atoms in a hexagonal lattice, [1] has captured extensive research interest due to its excellent mechanical, [2] thermal, [3] electronic, [1,4] and optical properties. [5,6] Due to its unique band structure, graphene shows ultrahigh carrier mobility, tunable transport polarity, and tunable broadband absorption, which make graphene a very promising candidate for use in electronic, photonic, and optoelectronic applications, such as transistors, [7] frequency multipliers, [8,9] frequency mixers, [10][11][1...