The study aims to improve the flexural behaviors of ultra-high performance fiber reinforced concrete (UHPFRC) by applying the concept of layered-structure. Deterministic criteria for layer cracking and debonding are proposed, formulas to predict the critical load at the first failure stage are developed, and effects of the layer E-modulus and thickness are assessed. Subsequently, double-layered UHPFRC beams are designed and tested under the three-point bending. Mechanical and interfacial properties of the beams are studied. Influences of the bottom layer thickness on the peak flexural load and the flexural energy are then investigated, which presents that a layer thickness ratio of 0.6 gives the optimum load carrying ability and beam flexural energy. The subsequent section discusses the effects of fiber re-arrangement on the flexural performances, revealing that the designed double-layered UHPFRC beam is able to withstand higher flexural load and energy than its single-layered counterpart with the same total fiber content. Moreover, it is exhibited that the peak flexural load is dependent on the fibers in the bottom layer while the flexural energy enhancement is related to fibers in both layers. The layered UHPFRC beam composed of a 40 mm-thick top layer with 0.6% steel fibers and a 60 mm-thick bottom layer with 1.6% fibers is an optimal choice leading to the superior peak flexural load and energy.