Unusual animal behaviors (UABs) have been observed before large earthquakes (EQs), however, their mechanisms are unclear. While information on UABs has been gathered after many EQs, few studies have focused on the ratio of emerged UABs or specific behaviors prior to EQs. On 11 March 2011, an EQ (Mw 9.0) occurred in Japan, which took about twenty thousand lives together with missing and killed persons. We surveyed UABs of pets preceding this EQ using a questionnaire. Additionally, we explored whether dairy cow milk yields varied before this EQ in particular locations. In the results, 236 of 1,259 dog owners and 115 of 703 cat owners observed UABs in their pets, with restless behavior being the most prominent change in both species. Most UABs occurred within one day of the EQ. The UABs showed a precursory relationship with epicentral distance. Interestingly, cow milk yields in a milking facility within 340 km of the epicenter decreased significantly about one week before the EQ. However, cows in facilities farther away showed no significant decreases. Since both the pets’ behavior and the dairy cows’ milk yields were affected prior to the EQ, with careful observation they could contribute to EQ predictions.