A facile sensor for selective differentiation and speciation of Fe 2+ and Fe 3+ , which are closely associated with cellular homeostasis and metabolism, was developed based on newly designed two-dimensional luminescent metalorganic frameworks (2D LMOFs). All the prepared LMOFs [Ln(TCPB) (DMF) 3 ] n (Ln = Tm, LMOF 1; Yb, LMOF 2; and Lu, LMOF 3; H 3 TCPB = 1,3,5-tris(1-(2-carboxyphenyl)-1H-pyrazol-3-yl)benzene) display strong tunable emissions by the adjustable metal-organic coordination interactions. The luminescence of LMOFs 1-3 can be quenched by Fe 3+ or oxidation of Fe 2+ through H 2 O 2 and recovered via reduction of Fe 3+ by ascorbic acid (AA). The mechanism for sensing Fe 3+ further demonstrates LMOF 1 with the highest sensitivity and the excellent selectivity. Besides, multiple logic gates were also constructed. This work represents a fast, accurate, and sensitive sensor integrated with logic operation capable of detecting Fe 3+ and intelligent discrimination and speciation of Fe 2+ and Fe 3+. The sensing system based on 2D LMOFs displays a convenient approach for developing sensing platforms with tunable luminescence.