Vertically aligned γ-AlOOH nanosheets (NSs) have been successfully fabricated on flexible Al foils via a solvothermal route without morphology-directing agents. Three different reaction temperature (25, 80, and 120 ◦C) and time (30 min, 45 min, and 24 h) are discussed for the growth period, which efficiently tune the density and size of the γ-AlOOH NSs. Meanwhile, the growth speed of the nanosheets confirms that dominant growth stage is seen in the initial 45 min. Furthermore, the interlayer of the γ-AlOOH NSs displays an average height of 140 nm and superhydrophilicity. By dynamic adsorption, the assynthesized γ-AlOOH NSs exhibit an outstanding NH3adsorption capacity of up to 146 mg/g and stably excellent regeneration for 5 cycles. The mechanism of NH3adsorption on the in-plane of the γ-AlOOH NSs is explained by the Lewis acid/base theory. The H-bond interactions among the NH3molecules and the edge groups (-OH) further improve the capture ability of the nanosheets.