The advent of the Internet of Things (IoT) has catalyzed 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 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 (LITEN). Employing Multivariate Metal−Organic Frameworks (MTV-MOFs), 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 with a minimal reflection loss of -50.6 dB at the optimal low-frequency C-band (around 4.98 GHz). Computational evidence reinforces GEMN’ efficacy in reducing radar cross sections. Additionally, GEMN demonstrates superior electromagnetic interference (EMI) shielding, reaching 98.92 dB in the THz band, with an average terahertz shielding of 55.47 dB (0.1~2THz). These accomplishments underscore GEMN's potential for 6G signal shielding. In summary, LITEN yields the remarkable EM wave 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.