anticounterfeiting, as well as bioimaging, biodetection, and thermal dynamic therapy. [7][8][9][10][11][12][13][14][15][16] In order to satisfy various functional parameters, large amount of efforts have been invested aiming to produce upconversion luminescence with expected characteristics in terms of the position, intensity, and lifetime of the emission bands, via suitable manipulations assisted by external stimuli, including electric field, magnetic field, temperature, mechanical force, as well as hydrostatic pressure. [17] Indeed, Hao et al. achieved a 2.7-fold upconversion luminescence enhancement by applying electric field on Yb 3+ / Er 3+ -doped epitaxially grown ferroelectric BaTiO 3 thin film, [18] Qiu et al. reported obvious luminescence enhancement under magnetic field in Yb 3+ /Ho 3+ -doped NaYF 4 nanoparticles, [19] Carlos et al. fabricated nanothermometers for precise and remote temperature sensing by taking advantage of temperature-induced upconversion luminescence emission, [20,21] and Xu et al. utilized mechanical luminescence generated by the fracture of constructions such as bridge, concrete wall, and buildings to monitor the status of constructions. [22,23] Compared to the above endeavors, hydrostatic pressure could offer unique merits to regulate and explore the luminescent properties, especially of upconversion luminescent materials, which is growing as a prevalent topic. [24][25][26] The tunable hydrostatic pressure can be utilized not only to probe the crystal structure and coordination bonding information of luminescent materials, but also to influence the electronic state and/or crystal field symmetry of luminescent ions. [27,28] This helps unveil the relationship between upconversion luminescent properties and crystal lattice variation of hosts, which provides direct insights in search of suitable crystal structures with improved performance for various purposes. [29] In addition, pressure-induced upconversion emission changes have wide applications in health monitoring, bioimaging, intelligent signature, optical sensors, nanomanometry, nanothermometry, [24,[30][31][32][33][34] as well as real-time monitoring of the working status of constructions via special coatings. [35][36][37][38] However, majority of such studies focused on downshifting luminescence and very limited examples targeted at upconversion emission whereas unfortunately, the unwanted decreased luminescence intensities are usually obtained under pressure. [24,25,34] The reason might be due to the Promising applications of downshifting mechanoluminescence have raised wide research enthusiasms in the past decades. However, weakened upconversion luminescence is usually obtained in lanthanide-doped materials under hydrostatic pressures. In layer-structured KAlF 4 , the z-axis has smaller elastic constant than that of the x-or y-axis, which can effectively tolerate high pressure influence on the coordination environment of luminescent ions by reducing the inter-layer distance and lead to enhanced upconversion luminescence. Ind...