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Since the low work function of ITO, introducing hole injection layer (HIL) with controllable and efficient property is an effective way to improve the performance of organic light-emitting diodes (OLEDs). In this work, films, containing molybdenum oxide units by employing H 2 O 2 treated ammonium phosphomolybdate (AMP) as precursors, are fabricated through solution-processed procedure. The hole injection property of the HILs can be modulated by the gap-state density, which is negatively correlated with the molar ratio of AMP/H 2 O 2. Green fluorescent and phosphorescent OLEDs based on the HILs are endowed with reduced turn-on voltage from 3.4 to 2.5 V and 4.1 to 3.4 V, respectively. Furthermore, fluorescent OLEDs based on the HIL with AMP/H 2 O 2 of 1:14 show a maximum current efficiency of 6.82 cd/A, 1.2-flod higher than that of PEDOT:PSS based devices. This method opens up a new path to obtain HIL with adjustable property in mild prepare condition for various electroluminescent devices. Image 1 • Controllable HILs with MoO 3 units were fabricated by solution-processed procedure. • Hole injection property of HILs was modulated by gap-state density, negatively correlated with AMP/H 2 O 2 molar ratio. • Green fluorescent and phosphorescent OLEDs based on the HILs were endowed with low turn-on voltage and high efficiency. [ABSTRACT FROM AUTHOR]