Inertial measurement units (IMUs) offer great opportunities to analyze segmental and joints kinematics. When combined with another motion capture system (MCS), for example, to validate new IMU-based applications or to develop mixed systems, it is necessary to align the local frame of the IMU sensors to the local frame of the MCS. Currently, all alignment methods use landmarks on the IMU's casing. Therefore, they can only be used with well-documented IMUs and they are prone to error when the IMU's casing is small. This study proposes an effortless procedure to align the local frame of any IMU to the local frame of any other MCS able to measure the orientation of its local frame. The general concept of this method is to derive the gyroscopic angles for both devices during an alignment movement, and then to use an optimization algorithm to calculate the alignment matrix between both local frames. The alignment movement consists of rotations around three more or less orthogonal axes and it can easily be performed by hands. To test the alignment procedure, an IMU and a magnetic marker were attached to a plate, and 20 alignment movements were recorded. The maximum errors of alignment (accuracy±precision) were 1.02°±0.32° and simulations showed that the method was robust against noise that typically affect IMUs. In conclusion, this study describes an efficient alignment procedure that is quick and easy to perform, and that does not require any alignment device or any knowledge about the IMU casing.