Two-dimensional (2D) materials have motivated widespread research interest due to their combination of atomic-scale, unique electromagnetic wave interactions and electronic properties. Advancements in several technologies, including portable and wireless electronics, are at the forefront of the developments. Developing low-dimensional materials is paramount for managing environmental electromagnetic pollution and enhancing the quality of communication within the shared limited bandwidths. However, step-by-step production and testing of low dimensional assemblies tailored for microwave absorption have rarely been reported, owing to their challenging synthesis. This work demonstrates how various losses can be effectively tuned using a complex 2D-MOFs nanoarray heterojunction structure. Firstly, low melting point liquid metals are used as reaction solvents, and their atomically thin interfaces are used to synthesize 2D Al(OH)3. The obtained 2D Al(OH)3 have been subsequently used as hydrothermal templates to construct unique Ni MOF derivative nanoarrays. Finally, nanocomposites are fabricated from the obtained low-dimensional materials. The unique morphology and nano-arrangement feature exceptional microwave absorption properties. The electromagnetic interactions have been fully characterized and an effective absorption bandwidth of 6.13 GHz can be achieved at 2.1 mm thickness of the fabricated nanocomposite. This work provides an avenue for exploring low dimensional morphologies and compositions for the production of high-quality electromagnetic wave nano-composites.