In order to harmonize robotic devices with human beings, the robots should be able to perceive important psychosomatic impact triggered by emotional states such as frustration or boredom. This paper presents a new type of biocooperative control architecture, which acts toward improving the challenge/skill relation perceived by the user when interacting with a robotic multimodal interface in a cooperative scenario. In the first part of the paper, open-loop experiments revealed which physiological signals were optimal for inclusion in the feedback loop. These were heart rate, skin conductance level, and skin conductance response frequency. In the second part of the paper, the proposed controller, consisting of a biocooperative architecture with two degrees of freedom, simultaneously modulating game difficulty and haptic assistance through performance and psychophysiological feedback, is presented. With this setup, the perceived challenge can be modulated by means of the game difficulty and the perceived skill by means of the haptic assistance. A new metric (FlowIndex) is proposed to numerically quantify and visualize the challenge/skill relation. The results are contrasted with comparable previously published work and show that the new method afforded a higher FlowIndex (i.e., a superior challenge/skill relation) and an improved balance between augmented performance and user satisfaction (higher level of valence, i.e., a more enjoyable and satisfactory experience).