The emergence of the internet of things has promoted wireless communication’s evolution towards multi-band and multi-area utilization. Notably, forthcoming sixth-generation (6G) communication standards, incorporating terahertz (THz) frequencies alongside existing gigahertz (GHz) modes, drive the need for a versatile multi-band electromagnetic wave (EMW) absorbing and shielding material. This study introduces a pivotal advance via a new strategy, called ultrafast laser-induced thermal-chemical transformation and encapsulation of nanoalloys (LITENs). Employing multivariate metal-organic frameworks, this approach tailors a porous, multifunctional graphene-encased magnetic nanoalloy (GEMN). By fine-tuning pulse laser parameters and material components, the resulting GEMN excels in low-frequency absorption and THz shielding. GEMN achieves a breakthrough of minimum reflection loss of −50.6 dB in the optimal C-band (around 4.98 GHz). Computational evidence reinforces GEMN’s efficacy in reducing radar cross sections. Additionally, GEMN demonstrates superior electromagnetic interference shielding, reaching 98.92 dB under THz band (0.1–2 THz), with the mean value result of 55.47 dB. These accomplishments underscore GEMN’s potential for 6G signal shielding. In summary, LITEN yields the remarkable EMW controlling performance, holding promise in both GHz and THz frequency domains. This contribution heralds a paradigm shift in EM absorption and shielding materials, establishing a universally applicable framework with profound implications for future pursuits.