Very recently, a 3D framework design integrating complex VAN structures has drawn great research interest. [2,6,21,22] The 3D framework is generated by integrating the multilayer and VAN designs together-numerous vertical nanopillars connect with the lateral interlayers to form a 3D interconnected frame embedded in the matrix. This 3D framework design combines the lateral and vertical strain engineering within the film, exhibits both advantages of the multilayer and VAN designs, and achieves an unprecedented degree of control of the film strain and properties. [6,22] The 3D framework thin films were first demonstrated in La 0.7 Sr 0.3 MnO 3 (LSMO)-CeO 2 systems by inserting one to three layers of CeO 2 (or LSMO) interlayers into the LSMO-CeO 2 VAN counterparts and forming 3D CeO 2 (or LSMO) frameworks. [6] Later, the feasibility of this 3D framework concept was demonstrated in LSMO-ZnO system along with a study on the effect of the ZnO interlayer thickness, which was controlled from 0 to ≈10 nm and effectively tuned the magnetotransport performance of the 3D framework films. [22] The overall framework (i.e., the secondary interlayers) embedded in all the reported 3D thin films is homogeneous, such as CeO 2 , LSMO, and ZnO. [6,21,22] Studies on heterogeneous interlayers are still rare. Moreover, the interlayer and its interplay with the matrix material are crucial for the 3D frameworks, since the 3D frames consist of vertical nanopillars and lateral interlayers.To achieve a precise control on the 3D framework structures, understanding the role of the interlayer within the 3D framework is significant and necessary.In this work, a set of 3D framework thin films have been processed by inserting different lateral interlayers (M). These interlayers present different in-plane matching distances from LSMO as illustrated in Figure 1a. The interlayer M candidates are yttria-stabilized zirconia (YSZ, 8 mol% Y 2 O 3 + 92 mol% ZrO 2 ), CeO 2 , SrTiO 3 (STO), BaTiO 3 (BTO), and MgO. In the resulting 3D structures, all ZnO nanopillars connect with the lateral interlayer M and create a 3D heterogeneous frame embedded in the LSMO matrix. The role of the lateral interlayer in determining the 3D heterogeneous framework microstructure and magnetotransport properties is systematically studied. The aforementioned interlayer materials are selected for the following reasons: 1) the in-plane lattice matching To investigate the role of interlayers on the growth, microstructure, and physical properties of 3D nanocomposite frameworks, a set of novel 3D vertically aligned nanocomposite (VAN) frameworks are assembled by a relatively thin interlayer (M) sandwiched by two consecutively grown La 0.7 Sr 0.3 MnO 3 (LSMO)-ZnO VANs layers. ZnO nanopillars from the two VAN layers and the interlayer (M) create a heterogeneous 3D frame embedded in the LSMO matrix. The interlayer (M) includes yttria-stabilized zirconia (YSZ), CeO 2 , SrTiO 3 , BaTiO 3 , and MgO with in-plane matching distances increasing from ≈3.63 to ≈4.21 Å, and expected in-plane stra...