A method is disclosed for tailoring the thermoelectric response of a thermocouple to that desired by a user. The method comprises the steps of; (a) selecting a first thermoelectric material, (b) selecting a second thermoelectric material having dissimilar thermoelectric properties to the first thermoelectric material, a thermocouple formed from the first thermoelectric material and the second thermoelectric material having a known thermoelectric response, and (c) modifying the chemical composition of at least one of the first thermoelectric material and the second thermoelectric material to produce a thermocouple having a tailored thermoelectric response. In specific embodiments, the chemical composition may be modified by selectively depleting one or more chemical elements from the thermoelectric material or by selectively adding, or increasing the proportion of, one or more elements to the thermoelectric material.