Ultra-broadband frequency entangled biphotons have exceptionally short temporal duration and can achieve narrow Hong–Ou–Mandel (HOM) interference patterns, making them vital for quantum metrology applications. However, the bandwidth of previously demonstrated biphotons used for HOM interference has been limited to less than 400 nm, which is not wide enough to achieve ultra-high precision in quantum metrology. In order to push the precision to its limit, we have theoretically designed a 20-mm-long chirped periodically poled lithium niobate (CPPLN) crystal with type-II phase matching. Pumped by a 405 nm laser, the down-converted signal and idler photons can cover the wavelength range from 420 to 5200 nm, approaching the transparent upper bound of the LN crystal. In the simulated Hong–Ou–Mandel (HOM) interference, the full-width at half-maximum of the interference pattern is 965 attoseconds, with a visibility of 99.44%. Following a similar approach, we also designed a type-0 CPPLN crystal to achieve higher brightness. These ultra-broadband biphoton sources can generate ultra-narrow quantum interference patterns, which have the potential for attosecond-level high-precision quantum metrology.