The knowledge of alloy–process–structure–property relationships is of particular interest for several safety-critical brazed components and requires a detailed characterization. Thus, three different nickel-based brazing filler metals were produced with varying chromium and molybdenum content and were used to braze butt joints of the austenitic stainless steel AISI 304L under vacuum. Two holding times were used to evaluate diffusion-related differences, resulting in six specimen variations. Significant microstructural changes due to the formation and location of borides and silicides were demonstrated. Using X-ray diffraction, alloy-dependent residual stress gradients from the brazing seam to the base material were determined and the thermal-induced residual stresses were shown through simulations. For mechanical characterization, impact tests were carried out to determine the impact toughness, as well as tensile tests at low and high strain rates to evaluate the strain-rate-dependent tensile strength of the brazed joints. Further thermal, electrical, and magnetic measurements enabled an understanding of the deformation mechanisms. The negative influence of brittle phases in the seam center could be quantified and showed the most significant effects under impact loading. Fractographic investigations subsequently enabled an enhanced understanding of the fracture mechanisms.