The free-standing protein matrix used here has two main advantages. The first is related to the molecular doping approach. It is well known that the BSA protein can bind a myriad of different molecules in a process we refer to as molecular doping. We showed previously that this process can induce long-range electron transport across the doped mat. The second advantage is having a solid-state free-standing biopolymer that contains large (>100 wt.%) water content. Thus, the resultant free-standing mat can be measured in a solid-state two-terminal device configuration, as described in this paper, and at the same time eliminating the need for an electrochemical setup though the photocurrent mechanism is identical to the one in electrochemical cells. At last, the artificial nature of our system, as opposed to natural systems, allows us to modulate its properties easily, and we show the manner in which the gradient doping of the Chl into the mat can change its light responsiveness. The solid-state 2-electrode configuration, together with the possibility of forming gradients of the molecular dopant, results in a simple polarization-dependent photocurrent device. We also show that other chromophores (those that nature does not use for light harvesting) can be molecularly doped into the mat, resulting in similar light responsiveness of the system. All in all, the free-standing protein matrices presented here represent a new family of polymeric materials for light harvesting, and while the purpose of this study is not to target the making of an efficient organic solar cell, the concepts we present here can be utilized for the future integration of polymers in such devices, which are currently dominated by thin layers of organic semiconductors.